Resin moldings and conductive resin composition

ABSTRACT

A shaped resin article comprising a polyamide (A) (comprising at least two different polyamide components), a polyphenylene ether (B) and a partially hydrogenated block copolymer (C) (obtained by partially hydrogenating a block copolymer comprising an aromatic vinyl polymer block and a conjugated diene polymer block) including a block copolymer (C-1) having a number average molecular weight of from 200,000 to 300,000, wherein (A) is present as a continuous phase in which (B) is dispersed to form a dispersed phase, and (C) is present in the continuous phase of (A) and/or the dispersed phase of (B), wherein the surface area of the polyamide (A) exposed on the overall surface of the shaped resin article is at least 80%, based on the surface area of the shaped resin article. A conductive resin composition comprising a polyamide (A), a polyphenylene ether (B), a partially hydrogenated block copolymer (C) comprising an aromatic vinyl polymer block and a conjugated diene polymer block, a conductive carbonaceous material (D) and wollastonite particles (E).

BACKGROUND OF THE INVENTION

1. Field of the Invention

The present invention relates to a shaped resin article. Moreparticularly, the present invention is concerned with a shaped resinarticle comprising: a polyamide (A) comprising at least two differentpolyamide components, a polyphenylene ether (B), and a specificpartially hydrogenated block copolymer (C), wherein polyamide (A) ispresent as a continuous phase in which polyphenylene ether (B) isdispersed to form a dispersed phase, and partially hydrogenated blockcopolymer (C) is present in at least one phase selected from the groupconsisting of the continuous phase of polyamide (A) and the dispersedphase of polyphenylene ether (B), wherein polyamide (A) is exposed onthe surface of the shaped resin article so that the total area of thepolyamide (A) exposed on the surface of the shaped resin article is atleast 80%, based on the surface area of the shaped resin article. Theshaped resin article of the present invention is advantageous not onlyin that the shaped resin article has excellent matte surface, but alsoin that the shaped resin article has excellent strength of adhesion to acoating formed on the shaped resin article (which strength of adhesionis hereinafter, referred to simply as “coating adhesion strength”), andsuch a coating formed on the shaped resin article has excellentsharpness of an image reflected therein (i.e., the coating has excellentluster). The present invention is also concerned with a conductive resincomposition comprising: a polyamide (A), a polyphenylene ether (B), aspecific block copolymer (C), a conductive carbonaceous material (D),and wollastonite particles (E). By the use of the conductive resincomposition of the present invention, it becomes possible to produce ashaped article which is advantageous not only in that the shaped articlehas excellent matte surface, but also in that the shaped article hasexcellent coating adhesion strength, and a coating formed on the shapedarticle has excellent sharpness of an image reflected therein. Further,the produced shaped article has a satisfactorily low coefficient oflinear expansion, which is especially advantageous in the field of largeshaped articles, such as an automobile fender and an automobile backdoor. The shaped resin article of the present invention and the shapedarticle produced from the conductive resin composition of the presentinvention can be advantageously used in a wide variety of fields, e.g.,not only in a field of exterior parts for automobiles, but also in thefields of electric and electronic parts, parts of office automationmachines, mechanical parts, and electric and interior parts ofmotorcycles and automobiles.

2. Prior Art

Polyphenylene ethers not only have excellent mechanical properties,excellent electrical properties (such as dielectric constant anddielectric dissipation factor) and excellent heat resistance, but alsohave excellent dimensional stability. Therefore, polyphenylene ethershave been used in a wide variety of fields. However, the moldability ofa polyphenylene ether is poor. For improving the moldability of apolyphenylene ether, Examined Japanese Patent Publication No. Sho 45-997discloses a technique in which a polyamide is added to a polyphenyleneether, to thereby obtain a polyamide-polyphenylene ether alloy. Furthervarious new techniques relating to polyamide-polyether alloys areproposed in, for example, U.S. Pat. Nos. 431,508, 4,732,938 and4,659,760. Nowadays, polyamide-polyether alloys are used in a very widevariety of fields, such as exterior parts for automobiles.

Many of exterior parts of automobiles are usually coated. Therefore, inthe choice of a material for exterior parts of automobiles, the strengthof adhesion of a material to a coating (which strength of adhesion ishereinafter, referred to simply as “coating adhesion strength”) is animportant factor.

Conventionally, various techniques have been proposed for impartingcoating adhesion strength to a polyamide-polyphenylene ether alloy. Forexample, Unexamined Japanese Patent Application Laid-Open SpecificationNo. Hei 8-109324 (corresponding to U.S. Pat. No. 5,554,693) discloses atechnique in which a specific terpene phenol resin is added to apolyamide-polyphenylene ether alloy so as to improve the coatingadhesion strength of the alloy. Further, Unexamined Japanese PatentApplication Laid-Open Specification No. Hei 3-143571 discloses atechnique in which a shaped resin article is treated with a surfactant,thereby improving the coating adhesion strength of the shaped resinarticle without precoating of the shaped article with a primer.

However, each of the above-mentioned techniques poses a problem in thatan additive is used to improve the coating adhesion strength of thealloy, thereby causing disadvantages in that the heat resistance of thealloy gets lowered, and in that the coated shaped particle of the alloyabsorbs moisture. Therefore, there has been a market demand for atechnique for improving the coatability of a shaped resin articlewithout the use of an additive.

Further, as one of the properties which are required of large shapedarticles (such as an automobile fender and an automobile back door),there can be mentioned a low coefficient of linear expansion. In anautomobile, there is provided a gap between an automobile fender and adoor, which gap is necessary for opening and closing the door. When anautomobile fender is produced from a material having a high coefficientof linear expansion, a disadvantage is caused in that the size of theabove-mentioned gap changes depending on the ambient temperature.Therefore, it has been desired to improve the coefficient of linearexpansion of a material used for producing the above-mentioned largeshaped articles.

In general, the coefficient of linear expansion of a material can beimproved by adding an organic or inorganic filler. However, when anorganic or inorganic filler is added to a material, a shaped articleproduced from the material is disadvantageous not only in that theorganic or inorganic filler is likely to be biasedly present near thesurface of the shaped article, but also in that the coating adhesionstrength is lowered, and a coating formed on the shaped article has poorluster. Therefore, it has been desired to improve simultaneously thecoefficient of linear expansion and coating adhesion strength of ashaped article, and the luster of a coating formed on the shapedarticle.

SUMMARY OF THE INVENTION

In this situation, the present inventors have made extensive andintensive studies with a view toward developing, without the use of anyof the above-mentioned additives, a polyamide-polyphenylene ether alloywhich can be used for producing a shaped article which is advantageousnot only in that the shaped article has excellent matte surface, butalso in that the shaped article has excellent coating adhesion strength,and a coating formed on the shaped article has excellent sharpness of animage reflected therein. As a result, it has unexpectedly been foundthat the above-mentioned object can be achieved by a shaped resinarticle comprising a polyamide, a polyphenylene ether and a partiallyhydrogenated aromatic vinyl/conjugated diene block copolymer, whereinthe area of polyamide exposed on the surface of the shaped resin articleis increased to a specific level. Further, the present inventors havefound that an excellent shaped article can be produced, without the useof an additive, from a conductive resin composition comprising apolyamide (A), a polyphenylene ether (B), a specific block copolymer(C), a conductive carbonaceous material (D) and wollastonite particles(E). Specifically, a shaped article produced from the conductive resincomposition is advantageous not only in that the shaped article hasexcellent matte surface, but also in that the shaped article hasexcellent coating adhesion strength, and a coating formed on the shapedarticle has excellent sharpness of an image reflected therein. Further,such a shaped article has an advantageously low coefficient of linearexpansion. Based on these findings, the present invention has beencompleted.

Accordingly, it is an object of the present invention to provide ashaped resin article which is advantageous not only in that the shapedresin article has excellent matte surface, but also in that the shapedresin article has excellent coating adhesion strength, and a coatingformed on the shaped resin article has excellent sharpness of an imagereflected therein.

It is another object of the present invention to provide a conductiveresin composition which enables the production of a shaped resin articlewhich is advantageous in that the shaped article has excellent mattesurface, in that the shaped article has excellent coating adhesionstrength, and a coating formed on the shaped article has excellentsharpness of an image reflected therein, and in that the shaped articlehas an advantageously low coefficient of linear expansion.

The foregoing and other objects, features and advantages of the presentinvention will be apparent from the following detailed description andthe appended claims.

DETAILED DESCRIPTION OF THE INVENTION

According to the present invention, there is provided a shaped resinarticle comprising:

a polyamide (A) comprising at least two different polyamide components,

a polyphenylene ether (B), and

one or more partially hydrogenated block copolymers (C), eachindependently obtained by partially hydrogenating an unhydrogenatedblock copolymer comprising at least one aromatic vinyl polymer blockcomprised mainly of aromatic vinyl monomer units, and at least oneconjugated diene polymer block comprised mainly of conjugated dienemonomer units, the partially hydrogenated block copolymers (C) includingat least one partially hydrogenated block copolymer (C-1) having anumber average molecular weight of from 200,000 to 300,000,

wherein the polyamide (A) is present as a continuous phase in which thepolyphenylene ether (B) is dispersed to form a dispersed phase, and thepartially hydrogenated block copolymer (C) is present in at least onephase selected from the group consisting of the continuous phase of thepolyamide (A) and the dispersed phase of the polyphenylene ether (B),

wherein the polyamide (A) is exposed on the surface of the shaped resinarticle so that the surface area of the polyamide (A) exposed on theoverall surface of the shaped resin article is at least 80%, based onthe surface area of the shaped resin article.

For easier understanding of the present invention, the essentialfeatures and various preferred embodiments of the present invention areenumerated below.

1. A shaped resin article comprising:

-   -   a polyamide (A) comprising at least two different polyamide        components,    -   a polyphenylene ether (B), and    -   one or more partially hydrogenated block copolymers (C), each        independently obtained by partially hydrogenating an        unhydrogenated block copolymer comprising at least one aromatic        vinyl polymer block comprised mainly of aromatic vinyl monomer        units, and at least one conjugated diene polymer block comprised        mainly of conjugated diene monomer units, the partially        hydrogenated block copolymers (C) including at least one        partially hydrogenated block copolymer (C-1) having a number        average molecular weight of from 200,000 to 300,000,    -   wherein the polyamide (A) is present as a continuous phase in        which the polyphenylene ether (B) is dispersed to form a        dispersed phase, and the partially hydrogenated block        copolymer (C) is present in at least one phase selected from the        group consisting of the continuous phase of the polyamide (A)        and the dispersed phase of the polyphenylene ether (B),    -   wherein the polyamide (A) is exposed on the surface of the        shaped resin article so that the surface area of the        polyamide (A) exposed on the overall surface of the shaped resin        article is at least 80%, based on the surface area of the shaped        resin article.        2. The shaped resin article according to item 1 above, wherein        the polyamide (A) comprises at least two different polyamide        components having their respective different viscosities.        3. The shaped resin article according to item 1 above, wherein        the component (A) comprises polyamide 6,6 and a polyamide other        than polyamide 6,6.        4. The shaped resin article according to item 3 above, wherein        the polyamide other than polyamide 6,6 is polyamide 6.        5. The shaped resin article according to item 3 above, wherein        the polyamide other than polyamide 6,6 is a polyamide comprising        recurring units, each independently represented by the following        formula (1):    -   wherein each of R¹ and R² independently represents a C₃-C₁₄        alkylene group or a C₆-C₉ arylene group, with the proviso that        R¹ and R² are not simultaneously a C₆ alkylene group or a C₆        arylene group.        6. The shaped resin article according to item 1 above, wherein        the polyamide (A) comprises at least one polyamide component        having a terminal amino group content of from 1×10⁵ mol/g to        4×10⁵ mol/g.        7. The shaped resin article according to item 1 above, wherein        the polyphenylene ether (B) contains relatively high molecular        weight polyphenylene ether molecules, each independently having        a molecular weight of 200,000 or more, and relatively low        molecular weight polyphenylene ether molecules, each        independently having a molecular weight of 5,000 or less,        wherein the weight ratio of the relatively high molecular weight        polyphenylene ether molecules to the relatively low molecular        weight polyphenylene ether molecules is 0.35 or less.        8. The shaped resin article according to item 1 above, wherein        the polyphenylene ether (B) contains relatively high molecular        weight polyphenylene ether molecules, each independently having        a molecular weight of 200,000 or more, and relatively low        molecular weight polyphenylene ether molecules, each        independently having a molecular weight of 5,000 or less,        wherein the amount of the relatively low molecular weight        polyphenylene ether molecules and the amount of the relatively        high polyphenylene ether molecules are, respectively, 5% by        weight or less and 2% by weight or less, based on the weight of        the polyphenylene ether resin (B).        9. The shaped resin article according to item 1 above, wherein        the one or more partially hydrogenated block copolymers (C)        further include at least one partially hydrogenated block        copolymer (C-2) having a number average molecular weight of from        50,000 to 150,000.        10. The shaped resin article according to item 9 above, wherein        the at least one partially hydrogenated block copolymer (C-1)        and the at least one partially hydrogenated block copolymer        (C-2) collectively include:    -   at least one partially hydrogenated block copolymer having a        high aromatic vinyl monomer unit content, which is obtained by        partially hydrogenating an unhydrogenated block copolymer in        which the at least one aromatic vinyl polymer block is present        in an amount of from 60 to 90% by weight, based on the weight of        the unhydrogenated block copolymer, and    -   at least one partially hydrogenated block copolymer having a low        aromatic vinyl monomer unit content, which is obtained by        partially hydrogenating an unhydrogenated block copolymer in        which the at least one aromatic vinyl polymer block is present        in an amount of from 20 to less than 60% by weight, based on the        weight of the unhydrogenated block copolymer, and    -   wherein the total amount of the aromatic vinyl polymer blocks        present in the hydrogenated block copolymers (C-1) and (C-2) is        30 to 40% by weight, based on the total weight of the        hydrogenated block copolymers (C-1) and (C-2).        11. The shaped resin article according to item 1 above, which        further comprises at least one carbonaceous material (D)        selected from the group consisting of a conductive carbon black,        carbon fibers and carbon nanotubes, and which is produced by        melt-kneading a master-batch comprising the polyamide (A) having        dispersed therein the carbonaceous material (D) with the        polyphenylene ether (B), the one or more partially hydrogenated        block copolymers (C), and optionally at least one member        selected from the group consisting of an additional amount of        the polyamide (A) and an additional amount of the carbonaceous        material (D).        12. The shaped resin article according to item 1 above, which        further comprises (E) wollastonite particles having an average        particle diameter of from 2 to 9 μm.        13. The shaped resin article according to item 12 above, wherein        the wollastonite particles (E) have at least two different        aspect ratios.        14. The shaped resin article according to item 1 above, which is        a pellet.        15. The shaped resin article according to item 1 above, which is        an automobile exterior part.        16. A conductive resin composition comprising:    -   a polyamide (A),    -   a polyphenylene ether (B),    -   a block copolymer (C) comprising at least one aromatic vinyl        polymer block comprised mainly of aromatic vinyl monomer units,        and at least one conjugated diene polymer block comprised mainly        of conjugated diene monomer units,    -   a conductive carbonaceous material (D), and    -   wollastonite particles (E).        17. The conductive resin composition according to item 16 above,        which is produced by melt-kneading a masterbatch comprising the        polyamide (A) having dispersed therein the carbonaceous        material (D) with the polyphenylene ether (B), the one or more        partially hydrogenated block copolymers (C), the wollastonite        particles (E), and optionally at least one member selected from        the group consisting of an additional amount of the        polyamide (A) and an additional amount of the carbonaceous        material (D), and wherein the carbonaceous material (D) is at        least one member selected from the group consisting of a        conductive carbon black, carbon fibers and carbon nanotubes.        18. The conductive resin composition according to item 16 above,        wherein the wollastonite particles (E) have an average diameter        of from 2 to 9 μm.        19. The conductive resin composition according to item 16 above,        wherein the wollastonite particles (E) include particles having        an aspect ratio of 5 or more and particles having an aspect        ratio of less than 5, wherein the amount of the wollastonite        particles (E) having an aspect ratio of 5 or more is 50% by        weight or more, based on the total weight of the wollastonite        particles (E).

Hereinbelow, the present invention is described in detail.

In one embodiment of the present invention, there is provided a shapedresin article comprising:

-   -   a polyamide (A) comprising at least two different polyamide        components,    -   a polyphenylene ether (B), and one or more specific partially        hydrogenated block copolymers (C),    -   wherein the polyamide (A) is present as a continuous phase in        which the polyphenylene ether (B) is dispersed to form a        dispersed phase, and the partially hydrogenated block        copolymer (C) is present in at least one phase selected from the        group consisting of the continuous phase of the polyamide (A)        and the dispersed phase of the polyphenylene ether (B),    -   wherein the polyamide (A) is exposed on the surface of the        shaped resin article so that the surface area of the        polyamide (A) exposed on the overall surface of the shaped resin        article is at least 80%, based on the surface area of the shaped        resin article.

With respect to the type of polyamide (A) which can be used in theshaped resin article of the present invention, there is no particularlimitation so long as it is a polymer having amide {—NH—C(═O)—} linkagesin the recurring units thereof.

In general, a polyamide is obtained by, for example, a ring openingpolymerization of a lactam, a condensation polymerization of a diamineand a dicarboxylic acid, or a condensation polymerization of anω-aminocarboxylic acid. However, in the present invention, the methodfor obtaining a polyamide is not limited to these examples.

Examples of diamines mentioned above include aliphatic diamines,alicyclic diamines and aromatic diamines. Specifically, there can bementioned tetramethylenediamine, hexamethylenediamine,undecamethylenediamine, dodecamethylenediamine, tridecamethylenediamine,2,2,4-trimethylhexamethylenediamine,2,4,4-trimethylhexamethylenediamine, 5-methyl-nonamethylenediamine,1,3-bisaminomethylcyclohexane, 1,4-bisaminomethylcyclohexane,m-phenylenediamine, p-phenylenediamine, m-xylylenediamine andp-xylylenediamine.

Examples of dicarboxylic acids include aliphatic dicarboxylic acids,alicyclic dicarboxylic acids and aromatic dicarboxylic acids.Specifically, there can be mentioned adipic acid, suberic acid, azelaicacid, sebacic acid, dodecanoic diacid, 1,1,3-tridecanoic diacid,1,3-cyclohexane dicarboxylic acid, terephthalic acid, isophthalic acid,naphthalene dicarboxylic acid and a dimer acid.

Specific examples of lactams include ε-caprolactam, enanthlactam andω-laurolactam.

Further, specific examples of ω-aminocarboxylic acids includeε-aminocaproic acid, 7-aminoheptanoic acid, 8-aminooctanoic acid,9-aminononanoic acid, 11-aminoundecanoic acid, 12-aminododecanoic acidand 13-aminotridecanoic acid.

In the present invention, the polyamide may either be a homopolymerobtained from any of the above-mentioned compounds (i.e., lactams,diamines, dicarboxylic acids and ω-aminocarboxylic acids), or acopolymer obtained by subjecting a mixture of at least two types of theabove-mentioned compounds to a condensation polymerization.

In the present invention, it is also preferred to use a polyamideobtained by a method in which one or more of the above-mentionedcompounds (i.e., lactams, diamines, dicarboxylic acids andω-aminocarboxylic acids) are polymerized in a polymerization reactor tothereby obtain a low molecular weight oligomer, and the obtainedoligomer is subjected to further polymerization in an extruder or thelike, to thereby obtain a high molecular weight polymer.

Examples of polyamides which can be advantageously used in the presentinvention include polyamide 6, polyamide 6,6, polyamide 4,6, polyamide11, polyamide 12, polyamide 6,10, polyamide 6,12, polyamide 6/6,6,polyamide 6/6,12, polyamide MXD (m-xylylenediamine), 6, polyamide 6,T,polyamide 6,I, polyamide 6/6,T, polyamide 6/6,I, polyamide 6,6/6,T,polyamide 6,6/6,I, polyamide 6/6,T/6,I, polyamide 6,6/6,T/6,I, polyamide6/12/6,T, polyamide 6,6/12/6,T, polyamide 6/12/6,I and polyamide6,6/12/6,I. Further, it is also possible to use a polyamide productobtained by blending or copolymerizing a plurality of differentpolyamides using an extruder or the like.

In the shaped resin article of the present invention, as polyamide (A),it is necessary to use two or more different polyamide components, andit is preferred to use a mixture of two or more different types ofpolyamide components having different viscosities. As examples of suchpolyamide mixtures, there can be mentioned a polyamide mixturecontaining a polyamide component having a viscosity of 80 ml/g and apolyamide component having a viscosity of 150 ml/g, and a polyamidemixture containing a polyamide component having a viscosity of 120 ml/gand a polyamide component having a viscosity of 115 ml/g, wherein eachof the viscosities of the polyamide components is measured in accordancewith ISO307 in a 96% sulfuric acid. When a polyamide mixture containingpolyamide components having different viscosities is used as polyamide(A), it is preferred that the viscosity of the polyamide mixture is inthe range of from 90 to 130 ml/g, more advantageously from 100 to 125ml/g. Whether or not such a polyamide mixture has a viscosity within theabove-mentioned range can be confirmed by a method in which polyamidecomponents to be used in a polyamide mixture are dissolved in a 96%sulfuric acid in the same weight ratio as in the polyamide mixture to beprepared, thereby obtaining a solution of the polyamide components, andthe viscosity measurement is performed in accordance with ISO307 usingthe obtained solution of the polyamide components. As described below,by using a combination of polyamide components having differentviscosities, it becomes possible to improve the coating adhesionstrength of the shaped resin article without sacrificing the mechanicalproperties of the shaped resin article.

Further, in the present invention, it is preferred that at least one ofthe polyamide components is polyamide 6,6. The use of polyamide 6,6 asat least one of the polyamide components is advantageous, for example,in that it becomes possible to suppress the lowering of heat resistanceof the shaped resin article.

As a polyamide other than polyamide 6,6, it is preferred to usepolyamide 6 and/or a polyamide represented by the following formula (1):

-   -   wherein each of R¹ and R² independently represents a C₃-C₁₄        alkylene group or a C₆-C₉ arylene group, with the proviso that        R¹ and R² are not simultaneously a C₆ alkylene group or a C₆        arylene group.

Among these polyamides, it is preferred to use at least one polyamideselected from the group consisting of polyamide 4,6, polyamide 6,12,polyamide 6,6/6,I, polyamide 6,6/6,T, polyamide 6,6/6,I/6,T, polyamide9,T and polyamide 12,T, it is more preferred to use at least onepolyamide selected from the group consisting of polyamide 6,12,polyamide 6,6/6,I and polyamide 6,6/6,T, and it is most preferred to usepolyamide 6,12 and/or polyamide 6,6/6,I.

When a combination of polyamide 6,6 and a polyamide other than polyamide6,6 is used as polyamide (A), the amounts of polyamide 6,6 and thepolyamide other than polyamide 6,6 can be appropriately selected;however, the amount of polyamide 6,6 is preferably in the range of from99 to 30% by weight, more preferably from 90 to 45% by weight, mostpreferably from 80 to 50% by weight, based on the weight of polyamide(A).

Further, it is preferred that polyamide (A) used in the shaped resinarticle of the present invention comprises at least one polyamide havinga terminal amino group content of from 1×10⁵ to 4×10⁵ mol/kg, moreadvantageously from 2×10⁵ to 3×10⁵ mol/kg. In such a case, there is noparticular limitation with respect to the terminal carboxyl groupcontent; however, it is preferred that the terminal carboxyl groupcontent is at least 5×10⁵ mol/g or more, more advantageously from 6×10⁵to 13×10⁵ mol/kg.

With respect to the above-mentioned terminal group content(s), polyamide(A) may contain a polyamide component which has terminal groupcontent(s) outside the above-mentioned range(s) so long as at least oneof the polyamide components used as polyamide (A) has terminal groupcontent(s) within the above-mentioned range(s). Further, it is preferredto use polyamide 6,6 which has terminal group content(s) within theabove-mentioned range(s).

With respect to a method for adjusting the terminal group content(s) ofa polyamide, any conventional methods which are well known in the artcan be used. For example, there can be mentioned a method in which atleast one compound selected from the group consisting of a diamine, amonoamine, a dicarboxylic acid and a monocarboxylic acid is added to thereaction system of a polymerization for producing a polyamide so as toobtain a polyamide having a desired terminal group content(s).

Further, in the shaped resin article of the present invention, aconventional metal-containing stabilizer (used for improving the heatstability of a polyamide) as described in Unexamined Japanese PatentApplication Laid-Open Specification No. Hei 1-163262 (corresponding toU.S. Pat. No. 4,857,575) may be used without causing any problems.

Among the conventional metal-containing stabilizers, especiallypreferred are CuI, CuCl₂, copper acetate and cerium stearate. Alsopreferred are halogen salts of alkali metals, such as potassium iodideand potassium bromide. These metal-containing stabilizers can be usedindividually or in combination.

It is preferred that the metal-containing stabilizer is added topolyamide (A) in an amount of 0.001 to 1 part by weight, relative to 100parts by weight of polyamide (A).

Further, in the shaped resin article of the present invention, as astabilizer other than the above-mentioned metal-containing stabilizer, aconventional organic stabilizer can be used without causing anyproblems. Examples of organic stabilizers include hindered phenolantioxidants, such as Irganox 1098; phosphorus-type stabilizers againstprocessing heat, such as Irgafos 168; lactone-type stabilizers againstprocessing heat, such as HP-136; sulfur-type heat stabilizers; andhindered amine photostabilizers.

Among the above-mentioned organic stabilizers, preferred are hinderedphenol antioxidants, phosphorus-type stabilizers against processingheat, and a mixture thereof. The amount of the organic stabilizer ispreferably from 0.001 to 1 part by weight, relative to 100 parts byweight of polyamide (A).

Further, any of other conventional additives for a polyamide can be alsoadded to polyamide (A). Such additive(s) can be used in an amount ofless than 10 parts by weight, relative to 100 parts by weight ofpolyamide (A).

Examples of polyphenylene ethers (B) which can be used in the shapedresin article of the present invention include a homopolymer and acopolymer, each independently comprising a structural unit representedby the following formula:

wherein O represents an oxygen atom, and each R independently representsa hydrogen atom, a halogen atom, a primary or secondary C₁-C₃ loweralkyl group, a C₆-Cg aryl group, a C₁-C₃ haloalkyl group, a C₁-C₃aminoalkyl group, a C₁-C₃ hydrocarbyloxy group or a C₁-C₃halohydrocarbyloxy group (in which at least two carbon atoms are presentbetween the halogen atom and the oxygen atom).

Specific examples of polyphenylene ethers which can be used for theshaped resin article of the present invention includepoly(2,6-dimethyl-1,4-phenylene ether),poly(2-methyl-6-ethyl-1,4-phenylene ether),poly(2-methyl-6-phenyl-1,4-phenylene ether) andpoly(2,6-dichloro-1,4-phenylene ether). Further examples ofpolyphenylene ethers include a copolymer of 2,6-dimethylphenol andanother phenol (for example, a copolymer of 2,6-dimethylphenol with2,3,6-trimethylphenol and a copolymer of 2,6-dimethylphenol with2-methyl-6-butylphenol, which are described in Examined Japanese PatentApplication Publication No. Sho 52-17880 (corresponding to U.S. Pat. No.4,011,200)).

Among the above-mentioned polyphenylene ethers, preferred arepoly(2,6-dimethyl-1,4-phenylene ether), a copolymer of2,6-dimethylphenol with 2,3,6-trimethylphenol, and a mixture thereof.

With respect to the method for producing polyphenylene ether (B) used inthe shaped resin article of the present invention, there is noparticular limitation, and any conventional methods can be used. Forexample, there can be mentioned methods as described in U.S. Pat. Nos.3,306,874, 3,306,875, 3,257,357 and 3,257,358, Unexamined JapanesePatent Application Laid-Open Specification No. Sho 50-51197(corresponding to U.S. Pat. No. 3,929,930), Examined Japanese PatentApplication Publication No. Sho 52-17880, and Unexamined Japanese PatentApplication Laid-Open Specification No. Sho 63-152628 (corresponding toU.S. Pat. No. 4,011,200).

With respect to polyphenylene ether (B) which can be used in the shapedresin article of the present invention, the reduced viscosity (η_(sp/c))thereof is preferably in the range of from 0.15 to 0.70 dl/g, morepreferably from 0.20 to 0.60 dl/g, still more preferably from 0.40 to0.55 dl/g, as measured at 30° C. with respect to a 0.5 g/dl chloroformsolution of the polyphenylene ether.

The use of a mixture of two or more different types of polyphenyleneethers having different reduced viscosities as polyphenylene ether (B)is advantageous in that a balance of the melt fluidity and impactresistance of polyphenylene ether (B) can be improved. As examples ofsuch a mixture, there can be mentioned a mixture of a polyphenyleneether having a reduced viscosity of 0.45 dl/g or less and apolyphenylene ether having a reduced viscosity of 0.50 dl/g or more, anda mixture of a polyphenylene ether having a reduced viscosity of 0.40dl/g or less and a polyphenylene ether having a reduced viscosity of0.50 dl/g or more, but the polyphenylene ether mixtures are not limitedto those which are exemplified above.

Polyphenylene ether (B) used in the present invention may be in amodified form or may be in the form of a mixture of an unmodifiedpolyphenylene ether and a modified polyphenylene ether. It is especiallypreferred to use, as polyphenylene ether (B), a mixture of an unmodifiedpolyphenylene ether and a modified polyphenylene ether.

In the present invention, the “modified polyphenylene ether” means apolyphenylene ether which is modified with at least one modifiercompound having at least one unsaturated bond selected from the groupconsisting of a carbon-carbon double bond and a carbon-carbon triplebond and having at least one functional group selected from the groupconsisting of a carboxylic acid group, an acid anhydride group, an aminogroup, a hydroxyl group and a glycidyl group, and any of the modifiedpolyphenylene ethers described in WO02/094936 can be used.

The modified polyphenylene ether used for producing the shaped resinarticle of the present invention may be in the form of a powder orpellets; however, it is preferred that the modified polyphenylene etheris in the form of pellets.

When a mixture of an unmodified polyphenylene ether and a modifiedpolyphenylene ether is used, there is no particular limitation withrespect to the amount of the modified polyphenylene ether; however, theamount of the modified polyphenylene ether is preferably from 10 to 95%by weight, more preferably from 30 to 90% by weight, most preferablyfrom 45 to 85% by weight, based on the weight of polyphenylene ether(B).

With respect to the addition of the polyphenylene ether in theproduction of the shaped resin article of the present invention, it ispreferred that a part or all of polyphenylene ether (B) is added to akneading machine (such as an extruder) in the form of pellets which havebeen obtained by melt-kneading the polyphenylene ether (B), and theresultant is added to a reaction mixture. By adding polyphenylene ether(B) in the form of such pellets, it becomes possible to improve theself-conveying ability of the polyphenylene ether in the kneadingmachine (such as an extruder), thereby improving the production rate ofthe shaped resin article. In addition, the use of polyphenylene ether(B) in the form of the above-mentioned pellets has the followingadvantage. In general, when it is intended to improve the productionrate of a shaped resin article, efficiency of volatilization during theproduction becomes lowered. Therefore, when the obtained shaped article(e.g., pellets) is used for producing an ultimate molded article using amolding machine, the resultant molded article suffers silver streaks dueto the residence of the molten shaped article (e.g., pellets) in amolding machine. However, by the use of the polyphenylene ether in theform of pellets which have been obtained by melt-kneading thepolyphenylene ether, it becomes possible to suppress the occurrence ofsuch silver streaks.

Further, it is preferred that polyphenylene ether (B) used in the shapedresin article of the present invention has a specific molecular weight.Specifically, it is preferred that polyphenylene ether (B) comprises arelatively high molecular weight polyphenylene ether having a molecularweight of 200,000 or more and a relatively low molecular weightpolyphenylene ether having a molecular weight of 5,000 or less, andsatisfies the following requirements (I) and/or (II):

(I) a requirement that the weight ratio of the relatively high molecularweight polyphenylene ether to the relatively low molecular weightpolyphenylene ether is 0.35 or less; and/or

(II) a requirement that the amounts of the relatively low molecularweight polyphenylene ether and the relatively high molecular weightpolyphenylene ether are 5% by weight or less and 2% by weight or less,respectively, based on the weight of polyphenylene ether (B).

It is more preferred that both of the above-mentioned requirements (I)and (II) are satisfied. By adjusting the molecular weight ofpolyphenylene ether (B) so as to satisfy requirements (I) and/or (II),it becomes possible to further improve the coating adhesion strength ofthe shaped resin article.

The measurement of the molecular weights of the above-mentionedrelatively low molecular weight polyphenylene ether and the relativelyhigh molecular weight polyphenylene ether can be performed by a methodcomprising the following steps 1) to 3).

1) A shaped resin article in an amount sufficient for the molecularweight measurement is pulverized. Then, the resultant pulverized shapedresin article is immersed in chloroform, and a soluble component thereofis dissolved therein by an ultrasonic washer or the like, therebyobtaining a solution.

2) The solution obtained in step 1) is analyzed by a gel permeationchromatography (GPC) apparatus and an ultraviolet spectrometricdetector. From the resultant data, the molecular weight data is obtainedusing a calibration curve obtained with respect to standard polystyrenesamples.

3) The molecular weight data obtained in step 2) is processed by acommercially available GPC processing software, so as to determine theamounts of molecules having molecular weights within a specific range.

In the measurement, it is important to operate the ultravioletspectrometric detector at a wavelength where an absorption ascribed tothe block copolymer(s) is not observed, so as not to detect the blockcopolymer(s) which elutes concomitantly with polyphenylene ether fromthe solution.

(Measurement conditions: GPC apparatus: GPC SYSTEM 21, manufactured andsold by Showa Denko Co., Japan; detector: UV-41, manufactured and soldby Showa Denko Co., Japan; solvent: chloroform; temperature: 40° C.;columns: columns for the sample (K-G, K-800RL and K-800R) and columnsfor the reference (K-805L, 2 columns); flow rate: 10 ml/min; wavelengthused for detection: 283 nm; and pressure: 15 to 17 kg/cm².) The shapedresin article of the present invention may contain a styrene-containingthermoplastic resin in an amount of less than 50 parts by weight,relative to 100 parts by weight of the total of polyamide (A) andpolyphenylene ether (B).

Herein, a styrene-containing thermoplastic resin means at least oneresin selected from the group consisting of a polystyrene (homopolymer),a rubber-modified polystyrene (HIPS), a styrene-acrylonitrile copolymer(AS resin) and a styrene-rubbery polymer-acrylonitrile copolymer (ABSresin).

Further, any of the conventional stabilizers for a polyphenylene ethercan be used in the production of the shaped resin article of the presentinvention. Examples of conventional stabilizers include metal-containingstabilizers, such as zinc oxide and zinc sulfide; and organicstabilizers, such as a hindered phenol type stabilizer, a phosphoroustype stabilizer and a hindered amine type stabilizer. The amount of thestabilizer(s) is preferably less than 5 parts by weight, relative to 100parts by weight of polyphenylene ether (B).

Furthermore, any of the conventional additives for a polyphenylene ethercan be used in the production of the shaped resin article of the presentinvention in an amount of less than 10 parts by weight, relative to 100parts by weight of polyphenylene ether (B).

Next, an explanation is given with respect to the partially hydrogenatedblock copolymer (C) which can be used in the shaped resin article of thepresent invention.

The partially hydrogenated block copolymer (C) which can be used in theshaped resin article of the present invention is obtained by partiallyhydrogenating an unhydrogenated block copolymer comprising at least onearomatic vinyl polymer block comprised mainly of aromatic vinyl monomerunits, and at least one conjugated diene polymer block comprised mainlyof conjugated diene monomer units.

The partially hydrogenated block copolymer (C) includes at least onepartially hydrogenated block copolymer (C-1) having a number averagemolecular weight of from 200,000 to 300,000.

In the present invention, “an aromatic vinyl polymer block comprisedmainly of aromatic vinyl monomer units” means an aromatic vinyl polymerblock which contains aromatic vinyl monomer units in an amount of atleast 50% by weight, based on the weight of the aromatic vinyl polymerblock. It is preferred that the aromatic vinyl polymer block containsaromatic vinyl monomer units in an amount of 70% by weight or more, moreadvantageously 80% by weight or more, most advantageously 90% by weightor more, based on the weight of the aromatic vinyl polymer block.

Similarly, “a conjugated diene polymer block comprised mainly ofconjugated diene monomer units” means a conjugated diene polymer blockwhich contains conjugated diene monomer units in an amount of at least50% by weight, preferably 70% by weight or more, more preferably 80% byweight or more, most preferably 90% by weight or more, based on theweight of the conjugated diene polymer block.

The above-mentioned aromatic vinyl polymer block may be, for example, acopolymer block in which a small amount of conjugated diene monomerunits are randomly inserted between the aromatic vinyl polymer units.

Similarly, the above-mentioned conjugated diene polymer block may be,for example, a copolymer block in which a small amount of aromatic vinylmonomer units are randomly inserted between the conjugated diene monomerunits.

Specific examples of aromatic vinyl compounds used for forming thearomatic vinyl monomer units include styrene, α-methyl styrene and vinyltoluene. These compounds can be used individually or in combination.Among the above-exemplified compounds, styrene is especially preferred.

Specific examples of conjugated dienes used for forming the conjugateddiene monomer units include butadiene, isoprene, piperylene and1,3-pentadiene. These compounds can be used individually or incombination. Among the above-exemplified compounds, butadiene, isopreneand a mixture thereof are preferred.

With respect to the microstructure of the conjugated diene polymer blockof partially hydrogenated block copolymer (C), it is preferred that the1,2-vinyl bond content or the total content of the 1,2-vinyl bond andthe 3,4-vinyl bond is 5 to 80%, more advantageously 10 to 50%, mostadvantageously 15 to 40%.

With respect to the unhydrogenated block copolymer used for producingpartially hydrogenated block copolymer (C), it is preferred thataromatic vinyl polymer block (a) and conjugated diene polymer block (b)have a block configuration selected from the group consisting of a-b,a-b-a and a-b-a-b. The block copolymer may be a mixture of differentblock copolymers having the above-mentioned block configurations. Amongthe above-mentioned block configurations, a-b-a and a-b-a-b are morepreferred, and a-b-a is most preferred.

Further, it is necessary that the block copolymer used in the presentinvention be a partially hydrogenated block copolymer.

The “partially hydrogenated block copolymer” herein means a copolymerwhich is obtained by hydrogenating any of the above-mentionedunhydrogenated block copolymers wherein the degree of hydrogenation ofthe aliphatic double bonds in the conjugated diene polymer block is morethan 0% and less than 100%. The degree of hydrogenation of the partiallyhydrogenated block copolymer is preferably 50% or more and less than100%, more preferably 80% or more and less than 100%, most preferably98% or more and less than 100%.

Further, it is necessary that the partially hydrogenated block copolymercontained in the shaped resin article of the present invention include apartially hydrogenated block copolymer (C-1) having a number averagemolecular weight of from 200,000 to 300,000. When only a partiallyhydrogenated block copolymer having a number average molecular weight ofless than 200,000 is used, the disadvantage is that the coating adhesionstrength of the shaped resin article is lowered. On the other hand, whenonly a partially hydrogenated block copolymer having a number averagemolecular weight of more than 300,000 is used, the disadvantage is thatthe melt fluidity of the resin composition used for producing the shapedresin article is lowered.

In the present invention, the number average molecular weight ismeasured by a gel permeation chromatography (GPC) apparatus (GPC SYSTEM21, manufactured and sold by Showa Denko Co., Japan), using anultraviolet spectrometric detector (UV-41, manufactured and sold byShowa Denko Co., Japan) and a calibration curve obtained with respect tostandard polystyrene samples. (Measurement conditions: solvent:chloroform; temperature: 40° C.; columns: columns for the sample (K-G,K-800RL and K-800R) and columns for the reference (K-805L, 2 columns);flow rate: 10 ml/min; wavelength used for detection: 254 nm; andpressure: 15 to 17 kg/cm².) In the measurement of the number molecularweight, a low molecular weight component formed due to the deactivationof a polymerization catalyst may sometimes be detected, but such a lowmolecular weight component is ignored in the calculation of themolecular weight. In general, a correctly calculated molecular weightdistribution (weight average molecular weight/number average molecularweight ratio) is in the range of from 1.0 to 1.1.

In the shaped resin article of the present invention, as theabove-mentioned partially hydrogenated block copolymers (C), it ispossible to use a mixture of at least one partially hydrogenated blockcopolymer (C-1) having a number average molecular weight of from 200,000to 300,000 and at least one partially hydrogenated block copolymer (C-2)having a number average molecular weight of from 50,000 to 150,000. Byusing a mixture of partially hydrogenated block copolymers (C-1) and(C-2), it becomes possible to improve the coating adhesion strength ofthe shaped resin article, and the balance of the impact resistance andmelt fluidity of the resin composition used in the production of theshaped resin article.

When a mixture of at least one partially hydrogenated block copolymer(C-1) and at least one partially hydrogenated block copolymer (C-2) isused as partially hydrogenated block copolymers (C), it is preferredthat the at least one partially hydrogenated block copolymer (C-1) andthe at least one partially hydrogenated block copolymer (C-2)collectively include:

at least one partially hydrogenated block copolymer having a higharomatic vinyl monomer unit content, which is obtained by partiallyhydrogenating an unhydrogenated block copolymer in which the at leastone aromatic vinyl polymer block is present in an amount of from 60 to90% by weight, based on the weight of the unhydrogenated blockcopolymer, and

at least one partially hydrogenated block copolymer having a lowaromatic vinyl monomer unit content, which is obtained by partiallyhydrogenating an unhydrogenated block copolymer in which the at leastone aromatic vinyl polymer block is present in an amount of from 20 toless than 60% by weight, based on the weight of the unhydrogenated blockcopolymer,

wherein the total amount of the aromatic vinyl polymer blocks present inthe hydrogenated block copolymers (C-1) and (C-2) is 30 to 40% byweight, based on the total weight of the hydrogenated block copolymers(C-1) and (C-2).

By using such a mixture of at least one partially hydrogenated blockcopolymer having a high aromatic vinyl monomer unit content and at leastone partially hydrogenated block copolymer having a low aromatic vinylmonomer unit content, it becomes possible to obtain a shaped resinarticle which is improved in respect both of impact resistance andstiffness at high temperatures.

In such a case, it is especially preferred to use partially hydrogenatedblock copolymer (C-2) (having a number average molecular weight of from50,000 to 150,000) which has a high aromatic vinyl monomer unit content,and is obtained by partially hydrogenating an unhydrogenated blockcopolymer in which the aromatic vinyl polymer block(s) is present in anamount of from 60 to 90% by weight, based on the weight of theunhydrogenated block copolymer. Further, with respect to the partiallyhydrogenated block copolymer having the above-mentioned specific numberaverage molecular weight and the above-mentioned specific aromatic vinylpolymer block content, it is preferred to use a block copolymer having anumber average molecular weight and an aromatic vinyl polymer blockcontent such that the number average molecular weight of the aromaticvinyl polymer blocks becomes 20,000 or more.

The number average molecular weight of aromatic vinyl polymer blocks ofa block copolymer can be calculated from the number average molecularweight of the block copolymer mentioned above in accordance with thefollowing formula:Mn_((a))={Mn>a/(a+b)}/N

-   -   wherein Mn_((a)) represents the number average molecular weight        of the aromatic vinyl polymer blocks; Mn represents the number        average molecular weight of the block copolymer; “a” represents        the % by weight of the total of the aromatic vinyl polymer        blocks, based on the weight of the block copolymer; “b”        represents the % by weight of the total of the conjugated diene        polymer blocks, based on the weight of the block copolymer; and        N represents the number of the aromatic vinyl polymer blocks in        the block copolymer.

The above-mentioned partially hydrogenated block copolymer may be amixture of different block copolymers so long as each of the blockcopolymers does not adversely affect the properties of the shaped resinarticle of the present invention. For example, the block copolymer maybe a mixture of block copolymers having different block configurations,a mixture of block copolymers containing different aromatic vinylmonomer units, a mixture of block copolymers containing differentconjugated diene monomer units, a mixture of block copolymers havingdifferent 1,2-vinyl contents or different total contents of 1,2-vinylbond and 3,4-vinyl bond, a mixture of block copolymers having differentaromatic vinyl monomer unit contents, and a mixture of block copolymershaving different degrees of hydrogenation.

The above-mentioned unhydrogenated block copolymer can be produced byany conventional methods. The above-mentioned hydrogenation of anunhydrogenated block copolymer can also be performed by any conventionalmethods.

In the present invention, it is also preferred to use a modified orpartially modified block copolymer or a block copolymer premixed with anoil, which are described in WO02/094936.

The shaped resin article of the present invention may further comprise acarbonaceous material (D). By adding carbonaceous material (D), itbecomes possible to use the shaped resin article in application fieldswhere a shaped resin article is required to have conductivity.

Carbonaceous material (D) which can be used in the shaped resin articleof the present invention is a carbonaceous filler which is capable ofimproving the conductivity (i.e., lowering the volume resistivity) ofthe shaped resin article by addition thereof.

Among such carbonaceous materials, especially preferred are a conductivecarbon black, carbon fibers and carbon nanotubes. These carbonaceousmaterials can be used individually or in combination. As a conductivecarbon black which can be used in the present invention, there can bementioned the conductive carbon black described in WO01/081473. Examplesof commercially available conductive carbon blacks include Ketjen BlackEC and Ketjen Black EC600JD (each manufactured and sold by Ketjen BlackInternational Company, Japan). As an example of carbon fibers which canbe used in the present invention, there can be mentioned very finecarbon fibers described in WO94/023433. Carbon nanotubes, in a broadsense, are included in carbon fibers; however, in general, acarbonaceous material having a specific tubular structure is referred toas a “carbon nanotube”. In the present invention, the term “carbonnanotube” means carbonaceous fibers and the like having a hollowstructure, a small amount of branches and a fiber diameter of less than75 nm, as described in U.S. Pat. Nos. 4,663,230, 5,165,909, 5,171,560,5,578,543, 5,589,152, 5,650,370 and 6,235,674. Further, carbon nanotubesmay be in the form of a coil having a coil pitch of 1 μm or less. In thepresent invention, the carbon nanotubes may have either a single layerstructure or a multilayer structure. Further, the carbon nanotubes alsoinclude those which have a relatively large amount of branches, a hollowstructure and a fiber diameter of 75 nm or more. As an example ofcommercially available carbon nanotubes, there can be mentioned BNFIBRIL (manufactured and sold by Hyperion Catalysis International,U.S.A).

In the shaped resin article of the present invention, it is preferredthat the amount of carbonaceous material (D) is from 0.5 to 2.5% byweight, more advantageously from 1.0 to 2.0% by weight, based on theweight of the shaped resin article.

As a preferred method for incorporating carbonaceous material (D) intothe shaped resin article of the present invention, there can bementioned a method in which at least a portion of carbonaceous material(D) is dispersed in at least a portion of at least one member selectedfrom the group consisting of polyamide (A), polyphenylene ether (B) andpartially hydrogenated block copolymer (C) to obtain a masterbatch, andthe thus obtained masterbatch (having carbonaceous material (D)dispersed therein) is used in the production of the shaped resinarticle. More preferred is a method in which at least a portion ofcarbonaceous material (D) is dispersed in at least a portion ofpolyamide (A) to obtain a masterbatch, and the thus obtained masterbatchis used in the production of the shaped resin article. With respect tothe method for producing the above-mentioned masterbatch, there is noparticular limitation; however, most preferred is a method in which themasterbatch is produced by melt-kneading using an extruder.Specifically, there can be mentioned a method which uses a co-rotatingtwin-screw extruder having at least one first inlet and at least onesecond inlet which are, respectively, provided at an upstream portion(s)and a downstream portion(s) of the extruder, wherein the inside of theextruder is preheated to 250 to 300° C., and wherein a resincomponent(s), such as polyamide (A), is fed to the extruder from thefirst inlet(s), thereby melt-kneading the resin(s) at an upstreamportion of the extruder, while feeding carbonaceous material (D) to theextruder from the second inlet(s), thereby melt-kneading the resin(s)and carbonaceous material (D) at a downstream portion of the extruder.In this method, it is preferred that the resin temperature is less than340° C. The amount of carbonaceous material (D) contained in themasterbatch is preferably from 5 to 30% by weight, more preferably from8 to 25% by weight, based on the weight of the masterbatch.

With respect to the form of the above-mentioned masterbatch containingat least a portion of carbonaceous material (D), there is no particularlimitation, and the masterbatch may be in any form, such as a powder,pellets, a sheet, a strand, or a mass having an indefinite shape;however, it is preferred that carbonaceous material (D) is in the formof pellets.

As the above-mentioned masterbatch, there can be used a commerciallyavailable masterbatch. As an example of commercially availablemasterbatches, there can be mentioned a polyamide 66/carbon fibermasterbatch which is manufactured and sold by Hyperion CatalysisInternational, U.S.A (trade name: Polyamide66 with Fibril™ NanotubesRMB4620-00; carbon fiber content: 20% by weight).

The shaped resin article of the present invention may further containwollastonite particles (E). As wollastonite particles (E), it ispreferred to use wollastonite particles having an average particlediameter of from 2 to 9 μm and an aspect ratio of 5 or more. (Herein,the term “average particle diameter” means an equivalent sphericaldiameter which is measured and calculated by Sedigraph particle diameteranalyzer (model 5100; manufactured and sold by Micromeritics InstrumentCorporation, U.S.A) with respect to a solution obtained by adding 0.75 gof wollastonite particles to 45 ml of a 0.05% Calgon solution andsatisfactorily dispersing the wollastonite particles therein by anultrasonic washer; and the term “aspect ratio” means an aspect ratiowhich is calculated from the average diameter and average length asmeasured with respect to at least 5,000 wollastonite particles on aphotomicrograph taken by an electron scanning microscope.) Aswollastonite particles, it is more preferred to use a mixture of two ormore types of wollastonite particles having different aspect ratios.Specifically, there can be used a mixture of wollastonite particleshaving an aspect ratio of 5 or more and wollastonite particles having anaspect ratio of less than 5.

With respect to such a mixture of wollastonite particles havingdifferent aspect ratios, it is most preferred that the amount ofwollastonite particles having an aspect ratio of 5 or more is 50% byweight or more, based on the total weight of wollastonite particlescontained in the mixture (i.e., total weight of wollastonite particles(E)).

As examples of preferred methods for incorporating wollastoniteparticles (E) into the shaped resin article of the present invention,there can be mentioned a method in which wollastonite particles (E)together with polyphenylene ether (B) are added to other materials forproducing a shaped resin article, and the resultant mixture ismelt-kneaded to thereby obtain a shaped resin article; a method in whichwollastonite particles (E) together with polyamide (A) are added toother materials for producing a shaped resin article, and the resultantmixture is melt-kneaded to thereby obtain a shaped resin article; and amethod in which polyphenylene ether (B) and polyamide (A) aremelt-kneaded together, followed by addition of wollastonite particles(E) thereto, and the resultant mixture is further melt-kneaded tothereby obtain a shaped resin article. Among the above-mentioned threemethods, the third method is most preferred.

Further, from the viewpoint of improving the dispersibility and handlingproperty of wollastonite particles (E), wollastonite particles (E) maybe added in the form of a wollastonite-containing masterbatch which isobtained by dispersing wollastonite particles in at least a portion ofpolyamide (A) and/or at least a portion of hydrogenated block copolymer(C).

As examples of specific methods for producing the above-mentionedwollastonite-containing masterbatch, there can be mentioned thefollowing methods (1) to (3): (1) a method in which, in the productionof polyamide (A), a raw material monomer(s) for producing polyamide (A)is polymerized in the presence of wollastonite to thereby obtain awollastonite-containing masterbatch; (2) a method which uses anextruder, wherein polyamide (A) and/or partially hydrogenated blockcopolymer (C) are/is dry-blended with wollastonite, and the resultantmixture is melt-kneaded at a temperature within a range such thatpolyamide (A) and/or partially hydrogenated block copolymer (C) are/ismelted satisfactorily and heat decomposition of the polymer(s) does notoccur; and (3) a method which uses a twin-screw extruder having a firstinlet provided at an upstream portion and a second inlet provided at adownstream portion of the extruder, wherein polyamide (A) and/orpartially hydrogenated block copolymer (C) are/is fed to the extruderfrom the first inlet, while feeding wollastonite to the extruder fromthe second inlet. Among these methods, method (3) is most preferred.

Further, in the present invention, a compatibility agent may beincorporated into the shaped resin article during the productionthereof.

With respect to compatibility agents which can be used in the presentinvention, there is no particular limitation so long as it is an agentwhich can improve the physical properties of a polyamide-polyphenyleneether alloy. Specifically, the compatibility agent which can be used inthe present invention is a multi-functional compound which interactswith one or both of the polyphenylene ether and the polyamide. Theinteraction may be either a chemical interaction (e.g., grafting) orphysical interaction (e.g., change in surface properties of thedispersed phase).

Examples of compatibility agents which can be used in the production ofthe shaped resin article of the present invention include those whichare described in detail in Unexamined Japanese Patent Laid-OpenSpecification Nos. Hei 8-8869 (corresponding to EP 201,416) and Hei9-124926 (corresponding to EP 747,439). All of the conventionalcompatibility agents described in these patent documents can be used inthe present invention, and the compatibility agents can be usedindividually or in combination.

Among various conventional compatibility agents, especially preferredare maleic anhydride and derivatives thereof, maleic acid andderivatives thereof, citric acid and derivatives thereof, fumaric acidand derivatives thereof, and polyphenylene ether pellets which have beenmodified with any of these compounds.

The amount of the compatibility agent used in the present invention ispreferably from 0.01 to 25 parts by weight, relative to 100 parts byweight of the total of polyamide (A) and polyphenylene ether (B).

With respect to the form of compatibility agents which can be used inthe present invention, there is no particular limitation. However, fromthe viewpoint of ease in handling, it is preferred to use compatibilityagents in the form of relatively large particles rather than in the formof a powder formed of fine particles. Specifically, for example, when acompatibility agent having a pungent odor (e.g., maleic anhydride) isused, it is preferred that the compatibility agent is in the form ofrelatively large particles because the pungent odor thereof is reducedas compared to the case where the compatibility agent is in the form ofa powder formed of fine particles, so that the working environment isnot spoiled.

With respect to compatibility agents in the form of relatively largeparticles, the particle diameter thereof is preferably 1 mm or more,more preferably in the range of from 1 mm to 10 mm, most preferably from3 to 8 mm. When the particle diameter is 10 mm or less, there is nodanger of occurrence of any troubles with respect to the feeding of theparticles into an extruder.

In the shaped resin article of the present invention, polyamide (A) ispresent as a continuous phase in which polyphenylene ether (B) isdispersed to form a dispersed phase, and partially hydrogenated blockcopolymer (C) is present in at least one phase selected from the groupconsisting of the continuous phase of the polyamide (A) and thedispersed phase of the polyphenylene ether (B). When the shaped resinarticle has a composition such that polyamide (A) cannot form acontinuous phase, the coating adhesion strength of the shaped resinarticle becomes disadvantageously low. With respect to the dispersionstate of partially hydrogenated block copolymer (C) in the dispersedphase of polyphenylene ether (B), there is no particular limitation, andpartially hydrogenated block copolymer (C) may have amicrophase-separated structure as described in U.S. Pat. No. 5,109,052,or may be in the form of a mass.

In the shaped resin article of the present invention, it is requiredthat polyamide (A) be exposed on the surface of the shaped resin articleso that the surface area of polyamide (A) exposed on the overall surfaceof the shaped resin article is at least 80%, based on the surface areaof the shaped resin article. It is preferred that the above-mentionedsurface area of polyamide (A) exposed on the overall surface of theshaped resin article (hereinafter, the above-mentioned surface area ofpolyamide (A) is frequently referred to simply as “polyamide arearatio”) is 90% or more.

When the above-mentioned polyamide area ratio is less than 80%, thecoating adhesion strength of the shaped resin article becomesdisadvantageously low.

The polyamide area ratio can be measured as follows.

From a shaped resin article, a flat plate having a size of about 1cm×about 1 cm is cut out, and used as a sample for the measurement ofthe polyamide area ratio. (When the shaped resin article is in the formof a pellet, the pellet per se is used as the sample). The obtainedsample is immersed in a 10% aqueous solution of phosphotungstic acid ata temperature of from 20 to 80° C. for not more than 24 hours, tothereby dye the sample selectively at the polyamide portions thereof.

After dying of the sample, the dyed sample is recovered from the aqueoussolution, followed by washing with water and drying. A photomicrograph(backscattered electron image) (magnification: ×2,500) of the surface ofthe dyed sample is taken using a field-emission scanning electronmicroscope (FE-SEM) (model “S-4700”; manufactured and sold by Hitachi,Ltd., Japan), wherein the microscope is operated at an accelerationvoltage of 5 kV and the photomicrograph is taken at an angleperpendicular to the surface portion of the sample where the portion isobserved under the microscope.

In the obtained image, the polyamide portions dyed with tungsten assumea white color due to the electron reflection of tungsten, and the undyedportions assume a black color. Thus, in the obtained image, the portionsattributed to the polyamide exposed on the surface of the shaped resinarticle can be distinguished from other portions.

With respect to the thus obtained photomicrograph (backscatteredelectron image), the total area of white portions thereof is measuredusing an image analysis device (model name: Image-Pro PLUS ver.4.0;Media Cybernetics, Inc., U.S.A.), and the ratio of the total area of thewhite portions to the overall area of the photomicrograph of the sampleis obtained as the polyamide area ratio. (In the measurement of thetotal area of the white portions in the backscattered electron image,the threshold for monochromization of the image is determined asfollows. From the histogram of the color tone of the backscatteredelectron image, an intensity of a peak attributed to the color of whiteand an intensity of a peak attributed to the color of black aredetermined, and the mean value of the two intensities is used as thethreshold for monochromization.)

The polyamide area ratio is determined by observing at least 10different portions of the surface of shaped resin article, and theaverage value of respective polyamide area ratios of the observedportions is defined as the polyamide area ratio of the shaped resinarticle. The above-mentioned at least 10 portions to be observed areselected from portions near the center of the shaped resin article, butnot from any surface portion (such as a surface portion or thereabout,which surface portion corresponds to a point in the mold at which a flowof a molten resin in a mold stops (such a surface portion is, hereafter,referred to as a “flow-end portion”)) which is expected to have a smallamount of the polyamide as compared to other portions. Specifically, forexample, in the case where the shaped resin article is produced byinjection molding, the above-mentioned portions to be observed for themeasurement of the polyamide area ratio are selected as follows. When aportion of the shaped resin article corresponding to the gate of a mold(such a portion is, hereinafter, referred to as a “gate portion”) isdefined as a starting point, and the distance from the gate portion tothe flow-end portion is defined as 1, the polyamide area ratio ismeasured with respect to portions within a distance of from 0 to 0.8 asmeasured from the starting point.

Further, when the shaped resin article is in the form of strand cutpellets (i.e., pellets obtained by a method in which a strand which hasbeen extruded from an extruder is cooled in a water bath, followed bycutting), cross-sections obtained by cutting the strand are not regardedas parts of the surface of the shaped resin article at which thepolyamide area ratio is measured. That is, in the case of a strand cutpellet, the polyamide area ratio is measured with respect to surfaceportions of the pellet other than surface portions which arecross-sections obtained by cutting the strand.

In the present invention, it is required that the polyamide area ratiomeasured with respect to the overall surface of the shaped resin articlebe high for achieving excellent coating adhesion strength of the shapedresin article. When such a requirement is satisfied, the coatingadhesion strength of the shaped resin article is greatly improved ascompared to the coating adhesion strength of a shaped article formedfrom a polyamide alone or a polyphenylene alone.

The shaped resin article of the present invention is characterized inthat a resin (hereinafter, referred to as a “dispersed phase resin”)which forms the dispersed phase (i.e., polyphenylene ether (B) andoptionally partially hydrogenated copolymer (C)) is present in a mannersuch that the dispersed phase resin forms moderate concavo-convexportions on the surface of the shaped resin article, and suchconcavo-convex portions are coated with polyamide (A). By virtue of thischaracteristic, the shaped resin article exhibits excellent effects asmentioned above. For forming the moderate concavo-convex portions by thedispersed phase resin, it is necessary to increase the melt viscosity ofthe dispersed phase resin. On the other hand, for forming a desiredcoating of polyamide (A) on the concavo-convex portions, it is preferredthat the melt viscosity of polyamide (A) is low.

For sufficiently increasing the melt viscosity of the dispersed phaseresin so as to form moderate concavo-convex portions on the surface ofthe shaped resin article, it is necessary that the molecular weight ofpartially hydrogenated block copolymer (C) be high. Specifically, byusing the above-mentioned partially hydrogenated block copolymer (C-1)which has a number average molecular weight of from 200,000 to 300,000,it becomes possible to form moderate concavo-convex portions on thesurface of the shaped resin article.

When a polyamide having a low melt viscosity is used alone as polyamide(A), it becomes possible to obtain a high polyamide area ratio; however,a disadvantage is that the mechanical properties (e.g., impact strength)of the shaped resin article are lowered. On the other hand, when apolyamide having a high melt viscosity is used alone as polyamide (A),the mechanical properties of the shaped resin article are improved;however, a disadvantage is that the polyamide area ratio as measuredwith respect to the surface of the shaped resin article is lowered, sothat the coating adhesion strength is lowered. Therefore, for achievingboth of excellent mechanical properties and excellent coating adhesionstrength, it is necessary to use a mixture of two or more type ofpolyamides as mentioned above.

In the present invention, it is preferred that the melt viscosity (asmeasured at 290° C. and a shear rate of 1,000 sec⁻¹) of the dispersedphase resin (i.e., polyphenylene ether (B) and optionally partiallyhydrogenated block copolymer (C)) is 800 Pa·s or more, moreadvantageously 1,000 Pa·s or more.

On the other hand, it is preferred that the melt viscosity (as measuredat 290° C. and a shear rate of 1,000 sec⁻¹) of the resin forming thecontinuous phase (i.e., polyamide (A)) (hereinafter, referred to as a“continuous phase resin”) is less than 200 Pa·s, more advantageouslyless than 100 Pa·s.

Further, it is preferred that the ratio of the melt viscosity of thedispersed phase resin to the melt viscosity of the continuous phaseresin is 10 or more, more advantageously 20 or more.

The melt viscosities of the dispersed phase resin and the continuousphase resin can be measured as follows. For example, the melt viscosityof the dispersed phase resin can be measured by a method in which amaterial having the same composition as that of the dispersed phaseresin is subjected to extrusion molding to obtain pellets, and the meltviscosity of the obtained pellets is measured by a capillary rheometeror the like. The melt viscosity of the continuous phase resin can bemeasured by the same method as mentioned above. In the measurement ofmelt viscosity of each of the dispersed phase resin and the continuousphase resin, even when an additive (such as wollastonite) is intended tobe incorporated into the resin used in the shaped resin article, themeasurement of melt viscosity of the resin is conducted withoutincorporating the additive into the resin.

By adjusting the melt viscosity of the dispersed phase resin, the meltviscosity of the continuous phase resin and the dispersed phaseresin/continuous phase resin melt viscosity ratio to 800 Pa-s or more,less than 200 Pa·s and 10 or more, respectively, it becomes easy toimprove the above-mentioned polyamide area ratio, and to maintain a highcoating adhesion strength (which is one of the characteristics of theshaped resin article of the present invention).

In the present invention, it is preferred that the weight ratio of thedispersed phase resin to the continuous phase resin is less than 1.0,more advantageously 0.9 or less. When the weight ratio of the dispersedphase resin to the continuous phase resin is controlled to less than1.0, it becomes possible to improve stably the above-mentioned polyamidearea ratio. Further, when partially hydrogenated block copolymer (C) ispresent in the dispersed phase of polyphenylene ether (B), it ispreferred that the amount of polyphenylene ether (B) in the dispersedphase is from 50 to 90% by weight, based on the total weight of thedispersed phase. When the amount of polyphenylene ether in the dispersedphase is large, it becomes possible to lower the luster of the shapedresin article. Specifically, it is preferred that the amounts ofpolyamide (A), polyphenylene ether (B) and partially hydrogenated blockcopolymer (C) are 50 to 70% by weight, 25 to 45% by weight and 5 to 25%by weight, respectively, based on the total weight of polyamide (A),polyphenylene ether (B) and partially hydrogenated block copolymer (C).It is more preferred that the amounts of polyamide (A), polyphenyleneether (B) and partially hydrogenated block copolymer (C) are 50 to 60%by weight, 35 to 45% by weight and 5 to 15% by weight, respectively,based on the total weight of polyamide (A), polyphenylene ether (B) andpartially hydrogenated block copolymer (C).

The shaped resin article of the present invention is characterized inthat the polyamide area ratio is at least 80% even when the polyamidecontent of the shaped resin article is less than 80% by weight. (Thismeans that the ratio of the polyamide exposed on the overall surface ofthe shaped resin article is not necessarily the same as the ratio of thepolyamide present in the shaped resin article as a whole.) By virtue ofthis characteristic, it becomes possible to achieve a high coatingadhesion strength. Examples of methods for adjusting the polyamide arearatio to at least 80% include a method in which the melt viscosity ofthe continuous phase resin is suppressed to a level lower than that ofthe dispersed phase resin; and a method in which the amount of areaction product (graft polymer) of polyamide (A) with polyphenyleneether (B) is adjusted to an appropriate level.

Specific examples of methods for suppressing the melt viscosity of thecontinuous phase resin to a level lower than that of dispersed phaseresin include the above-mentioned method in which the viscosity ofpolyamide (A) is adjusted; a method in which the polymerization degreeof polyphenylene ether is adjusted so as to adjust the molecular weightof the polyphenylene ether (used in the shaped resin article) to fallwithin the above-mentioned range; and a method in which two or morepolyphenylene ethers having different molecular weights are blended.

Specific examples of methods for adjusting the amount of a reactionproduct (graft polymer) of polyamide (A) with polyphenylene ether (B) toan appropriate level include a method in which the above-mentionedpolyamide having the specific amino group content is used; and a methodin which the modification degree of the polyphenylene ether is adjusted(e.g., by mixing a modified polyphenylene ether with an unmodifiedpolyphenylene ether).

In the present invention, the method for adjusting the polyamide arearatio to at least 80% is not limited to those exemplified above.Further, a plurality of different methods may be used in combination foradjusting the polyamide area ratio.

With respect to the shaped resin article of the present invention, whenwollastonite is used, it is preferred that the amount of wollastonite issuch that the average coefficient of linear expansion of the shapedresin article is in the range of from 4.5×10⁻⁵° C.⁻¹ to 6.5×10⁻⁵° C.⁻¹,wherein the average coefficient of linear expansion of the shaped resinarticle is measured as follows. A type D2 flat plate having a thicknessof 2 mm (prescribed in ISO294-3:1996) is prepared under conditionsprescribed in ISO15103-2:1997 (melting temperature: 290° C., moldtemperature: 90° C.). Then, from the center of the type D2 flat plate iscut out a segment thereof having a size of 10 mm (length as measured inthe direction of flow of a resin in a mold)×3 mm (width as measured inthe direction perpendicular to the direction of flow of a resin in amold)×2 mm (thickness), and the resultant flat plate is allowed to standat 100° C. for at least 48 hours, to thereby obtain a test specimen.Using the obtained test specimen, the coefficient of linear expansion ismeasured in accordance with JIS K7197-1991 at a temperature of from −30to 80° C. at a temperature elevation rate of 5° C./min.

Specifically, the amount of wollastonite is preferably from 10 to 50parts by weight, more preferably 15 to 35 parts by weight, relative to100 parts by weight of the total of polyamide (A), polyphenylene ether(B) and partially hydrogenated block copolymer (C).

In the present invention, in addition to the above-mentioned componentsof the shaped resin article, if desired, an additional component(s) canbe incorporated into the shaped resin article so long as the additionalcomponent(s) does not adversely affect the excellent properties of theshaped resin article of the present invention.

Examples of additional components include thermoplastic resins otherthan mentioned above, such as a polyester and a polyolefin; inorganicfillers (such as talc, kaolin, xonotlite, titanium oxide, potassiumtitanate, a carbon fiber and a glass fiber); conventional silanecoupling agents which enhance the affinity between an inorganic fillerand a resin; flame retardants (such as a halogenated resin, a siliconeflame retardant, magnesium hydroxide, aluminum hydroxide, an organicphosphoric ester compound, ammonium polyphosphate and red phosphorus),fluororesins having an effect to prevent the dripping of flamingparticles; plasticizers (such as an oil, a low molecular weightpolyolefin, a polyethylene glycol and a fatty ester); auxiliary flameretardants, such as antimony trioxide; carbon black as a pigment;conductivity-imparting agents, such as a carbon fiber and a conductivecarbon black; antistatic agents; various peroxides; antioxidants;ultraviolet absorbers; and light stabilizers.

In the present invention, the amount of the additional component(s)incorporated into the shaped resin article is not more than 100 parts byweight, relative to 100 parts by weight of the total weight of polyamide(A), polyphenylene ether (B), partially hydrogenated block copolymer (A)and the compatibility agent.

Next, explanation is given below with respect to the method forproducing a resin composition which can be used for producing the shapedresin article of the present invention.

As specific examples of processing apparatuses which can be used toprepare the above-mentioned resin composition of the present invention,there can be mentioned a single-screw extruder, a twin-screw extruder, aroll, a kneader, a Brabender Plastograph and a Banbury mixer. Amongthese apparatuses, preferred is a twin-screw extruder, and especiallypreferred is a twin-screw extruder provided with a first inlet and atleast one second inlet which are, respectively, formed at an upstreamportion and a downstream portion of the extruder.

It is especially preferred to use an extruder having a screw diameter of50 mm and equipped with 3 or more feeders, wherein a polyamide, apolyphenylene ether and a compatibility agent are fed to the extruder bydifferent feeders, respectively, thereby melt-kneading together thepolyamide, the polyphenylene ether and the compatibility agent.

Especially when the compatibility agent used is in the form ofrelatively large particles, and the polyphenylene ether used is in theform of a powder formed of fine particles, the use of different feedersfor the feeding of the compatibility agent and the feeding of thepolyphenylene ether is advantageous in that it becomes possible toprevent the classification of the particle mixture (i.e., mixture ofrelatively large particles of the compatibility agent and fine particlesof the polyphenylene ether) in an extruder, which classification leadsto a disadvantage in that the ratio of the compatibility agent to thepolyphenylene ether varies depending on a position in a feeder used forfeeding both of the compatibility agent and the polyphenylene ether.When such a disadvantage is caused, the ratio of the polyphenylene etherto the compatibility agent, which are fed to the extruder, fluctuatesduring the operation of the extruder, thereby causing the fluctuation ofthe viscosity and particle diameter of the dispersed phase resin. Such afluctuation of the viscosity and particle diameter of the dispersedphase resin is likely to cause a problem in that the luster and coatingadhesion strength of the final shaped resin article varies depending ona position in the shaped resin article.

Further, as a feeder for the compatibility agent, it is especiallypreferred to use a screw-type gravimetric feeder. By using a screw-typegravimetric feeder, the stability of the feeding of the compatibilityagent is improved, thereby suppressing the fluctuation of the quality ofthe final shaped resin article.

With respect to the melt-kneading temperature used for producing theresin composition, there is no particular limitation. In general, anappropriate temperature for obtaining a desired resin composition isselected from the range of from 240 to 360° C. The resin temperatureduring the melt-kneading is preferably from 310 to 340° C.

Specific examples of the method for producing the above-mentioned resincomposition are described below. However, needless to say, the methodfor producing the above-mentioned resin composition should not belimited to these examples.

As an apparatus used for producing the resin composition, there can bementioned a twin-screw extruder having a first inlet and at least onesecond inlet which are provided, respectively, at upstream anddown-stream portions of the extruder, wherein the first inlet isprovided with a screw-type gravimetric feeder and a belt-typegravimetric feeder, and the second inlet is provided with anotherscrew-type gravimetric feeder. Using such a twin screw extruder, theproduction of the resin composition can be performed by any of thefollowing methods (1) to (3): (1) a method in which a mixture of a blockcopolymer and a polyphenylene ether is fed to the extruder from thefirst inlet by the belt-type gravimetric feeder, and a compatibilityagent is fed to the extruder through the first inlet by the screw-typegravimetric feeder, thereby melt-kneading together the above-mentionedmixture and the compatibility agent at the upstream portion of theextruder, while feeding a polyamide to the extruder from the secondinlet, thereby melt-kneading the resultant mixture at the downstreamportion of the extruder; (2) a method in which a polyphenylene ether isfed to the extruder from the first inlet by the belt-type gravimetricfeeder, and a mixture of a compatibility agent and a block copolymer isfed to the extruder from the first inlet by the screw-type gravimetricfeeder, thereby melt-kneading together the polyphenylene ether and theabove-mentioned mixture, while feeding a polyamide to the extruder fromthe second inlet, thereby melt-kneading the resultant mixture at thedownstream portion of the extruder; and (3) a method in which apolyphenylene ether in the form of a powder is fed to the extruder fromthe first inlet by the belt-type gravimetric feeder, and a compatibilityagent and a polyphenylene ether in the form of pellets are fed to theextruder from the first inlet by the screw-type gravimetric feeder,thereby melt-kneading together the polyphenylene ether and thecompatibility agent, while feeding a polyamide to the extruder from thesecond inlet, thereby melt-kneading the resultant mixture at thedownstream portion of the extruder.

The thus produced resin composition is subjected to molding by a desiredmethod, thereby obtaining the shaped resin article of the presentinvention. The shaped resin article includes not only injection-moldedarticles, but also extrusion-molded articles, such as sheets, films andpellets, and secondary processed molded articles which are obtained bysubjecting the above-mentioned extrusion-molded articles to injectionmolding or the like. Preferred examples of the forms of the shaped resinarticle include cylindrical pellets, each having a diameter of less than3 mm and a length of less than 3 mm; spherical pellets, each having adiameter of less than 3 mm; disc-shaped pellets, each having a diameterof less than 4 mm; and an injection-molded article obtained bysubjecting any one of the above-mentioned pellets to injection molding.

In another aspect of the present invention, there is provided aconductive resin composition comprising:

-   -   a polyamide (A),    -   a polyphenylene ether (B),    -   a block copolymer (C) comprising at least one aromatic vinyl        polymer block comprised mainly of aromatic vinyl monomer units,        and at least one conjugated diene polymer block comprised mainly        of conjugated diene monomer units,    -   a conductive carbonaceous material (D), and    -   wollastonite particles (E).

With respect to polyamide (A) used in the conductive resin compositionof the present invention, any of the polyamides which are describedabove in connection with the shaped resin article of the presentinvention can be used. However, in the conductive resin composition ofthe present invention, it is not necessary to use two or more differenttypes of polyamides, and only one type of polyamide may be used aspolyamide (A). Nevertheless, it is preferred to use two or moredifferent types of polyamides as in the case of the shaped resin articleof the present invention.

With respect to polyphenylene ether (B) used in the conductive resincomposition of the present invention, any of the polyphenylene etherswhich are described above in connection with the shaped resin article ofthe present invention can be used.

Further, with respect to block copolymer (C) used in the conductiveresin composition of the present invention, any of the block copolymerswhich are described above in connection with the shaped resin article ofthe present invention can be used. However, block copolymer (C) used inthe conductive resin composition of the present invention does not needto be hydrogenated.

It is preferred that block copolymer (C) used in the conductive resincomposition of the present invention has a number average molecularweight in the range of from 50,000 to less than 150,000.

Furthermore, with respect to conductive carbonaceous material (D) andwollastonite particles (E), any of the conductive carbonaceous materialsand wollastonite particles which are described above in connection withthe shaped resin article of the present invention can be used.

With respect to the method for producing the conductive resincomposition of the present invention, any of the methods which aredescribed above in connection with the resin composition that can beused for producing the shaped resin article of the present invention canbe used.

Examples of various molded articles which can be produced from theshaped resin article and conductive resin composition of the presentinvention include electric equipment for motorcycles and automobiles,such as a relay box material; parts for electric or electronicappliances, such as an IC tray, a chassis and cabinet of various discplayers; parts for office automation machines and mechanical parts, suchas various computers and peripheral equipment therefor; parts formotorcycles, such as a cowl; exterior parts for automobiles, such as abumper, a fender, a door panel, various moles and emblems for anautomobile, an outer door handle, a door mirror housing, a wheel cap, aroof rail and a staying material therefor, and a spoiler; and interiorparts for automobiles, such as an instrument panel, a console box and atrim.

Among the above-exemplified molded articles, the shaped resin articleand conductive resin composition of the present invention are suitablefor producing exterior parts for automobiles.

BEST MODE FOR CARRYING OUT THE INVENTION

Hereinbelow, the present invention will be described in more detail withreference to the following Production Examples, Examples and ComparativeExamples, which should not be construed as limiting the scope of thepresent invention.

PRODUCTION EXAMPLE 1 Production of Polyphenylene Ether Modified withMaleic Anhydride (Hereinafter, Referred to as “MPPE”)

MPPE was prepared as follows. 3 Parts by weight of maleic anhydride and100 parts by weight of polyphenylene ether having a reduced viscosity of0.42 dl/g were dry blended, followed by melt-kneading and subsequentpelletization in an extruder “ZSK-40” (manufactured and sold by CoperionWerner & Pfleiderer GmbH & Co. KG, Germany; L/D (the ratio of the length(L) of the screw of the extruder to the diameter (D) of the screw of theextruder)=42) at a cylinder temperature of 320° C., thereby obtainingMPPE in the form of pellets.

PRODUCTION EXAMPLE 2 Production of a Copolymer of Polyamide 6,6 andPolyamide 6,I (Hereinafter, Abbreviated to “PA66/6I”)

Into an autoclave having a volume of 50 liters were charged 20.0 kg ofan equimolar salt of adipic acid and hexamethylenediamine, 5.0 kg of anequimolar salt of isophthalic acid and hexamethylenediamine, 1.0 kg ofadipic acid and 25 kg of purified water. The contents of the autoclavewere well stirred, and the atmosphere inside the autoclave was fullypurged with nitrogen. Subsequently, the temperature of the autoclave waselevated from room temperature to 220° C. over about 1 hour whilestirring.

During the elevation of the temperature of the autoclave, the internalpressure increased due to the natural pressure increase caused by thesteam inside the autoclave; however, the heating of the autoclave wasperformed while removing the water from the reaction system in theautoclave so as to prevent the internal pressure of the autoclave fromexceeding 18 kg/cm²-G. After the temperature of the autoclave reached220° C., the heating of the autoclave was continued for two hours toelevate the temperature to 260° C., whereupon the heating was stopped.Subsequently, the discharge bulb of the autoclave was closed, and theautoclave was allowed to cool to room temperature over about eighthours. Then, the autoclave was opened, and 20 kg of a polymer was takenout from the autoclave. The polymer was pulverized, thereby obtaining apulverized polymer.

The thus obtained pulverized polymer was subjected to a solid phasepolymerization at 200° C. for 10 hours under a flow of nitrogen gas, toobtain a polyamide.

The thus obtained polyamide had a hexamethylene isophthalamide monomerunit content of about 19 mol %, a terminal amino group content of3.9×10⁵ mol/g and a terminal carboxyl group content of 10.2×10⁵ mol/gper kg of the polyamide.

PRODUCTION EXAMPLE 3 Production of a Polyamide/Carbon Masterbatch(Hereinafter, Referred to as “PA-MB”)

PA-MB was produced using a twin-screw extruder (ZSK-58MC, manufacturedand sold by Coperion Werner & Pfleiderer GmbH & Co. KG, Germany) whichhad one inlet at an upstream portion thereof (hereinafter, referred toas “upstream inlet”) and another inlet at a downstream portion thereof(hereinafter, referred to as “downstream inlet”), wherein L/D (the ratioof the length (L) of the screw of the extruder to the diameter (D) ofthe screw of the extruder) was 46. Specifically, into the twin-screwextruder were introduced 90 parts by weight of PA66-1 and 10 parts byweight of KB (i.e., ketjen black) through the upstream inlet of theextruder and the downstream inlet of the extruder, respectively. Thecontents of the extruder were melt-kneaded under conditions wherein thecylinder temperatures were 280° C. at a portion between the upstreaminlet and the downstream inlet of the extruder, and 300° C. at a portionbetween the downstream inlet and the dye, the screw revolution rate was400 rpm and the discharge rate was 300 kg/h, to thereby produce PA-MB.

EXAMPLE 1

Pellets of a resin composition were produced using a co-rotatingintermeshing twin-screw extruder “ZSK-70MC” (manufactured and sold byCoperion Werner & Pfleiderer GmbH & Co. KG, Germany; L/D=46) which hastwelve cylinder units (which are, respectively, referred to as “1stcylinder unit”, “2nd cylinder unit” . . . “12th cylinder unit” as viewedin an extrusion direction of the extruder) and a dye, wherein therespective temperatures of the cylinder units can be separatelyadjusted. The extruder has an inlet at the 1st cylinder unit(hereinafter, referred to as “upstream inlet”), another inlet at the 6thcylinder unit (hereinafter, referred to as “1st downstream inlet”),still another inlet at the 8th cylinder unit (hereinafter, referred toas “2nd downstream inlet”), and two vent ports (through which vacuumsucking can be performed) at the 5th and 11th cylinder units. A belttype gravimetric feeder and two screw type gravimetric feeders areprovided at the upstream inlet of the extruder, and another screw typegravimetric feeder is provided at the 1st downstream inlet of theextruder.

Specifically, using the above-mentioned extruder, the production ofpellets of a resin composition was performed as follows. First, rawmaterials for the resin composition were fed to the above-mentionedextruder as follows. A polyphenylene ether powder (hereinafter, referredto as “PPE1”) having a reduced viscosity of 0.52 dl/g (as measured withrespect to a chloroform solution thereof having a polyphenylene etherconcentration of 0.5 g/dl at 30° C.) was fed to the extruder through oneof the screw type gravimetric feeders (hereinafter, referred to as“feeder 1”) provided at the upstream inlet of the extruder. Maleicanhydride (in the form of tablets each having a diameter of 4 to 5 mm)(manufactured and sold by Mitsubishi Chemical Corporation, Japan)(hereinafter, abbreviated to “MAH”) as a compatibilizer was fed to theextruder through the other screw type gravimetric feeder (hereinafter,referred to as “feeder 2”) provided at the upstream inlet of theextruder. 4 Parts by weight of a polystyrene/polyethylenebutylene/polystyrene block copolymer (styrene content: 33%)(hereinafter,referred to as “SEBS1”) having a number average molecular weight (Mn) of246,000 and 8 parts by weight of a polystyrene/polyethylenebutylene/polystyrene block copolymer (styrene content: 29%)(hereinafter,referred to as “SEBS2”) having a number average molecular weight (Mn) of98,500 were dry blended using a Henschel mixer. The resultant mixturewas fed to the extruder through the belt type gravimetric feeder(hereinafter, referred to as “feeder 3”) provided at the upstream inletof the extruder. By using a tumbler, a polyamide blend was prepared bydry blending 40 parts by weight of polyamide 6,6 (hereinafter, referredto as “PA66-a”) having a viscosity number of 120 ml/g, a terminal aminogroup content of 2.5×10⁵ mol/g and a terminal carboxyl group content of11.6×10⁵ mol/g, with 10 parts by weight of polyamide 6,6 (hereinafter,referred to as “PA66-b”) having a viscosity number of 130 ml/g, aterminal amino group content of 4.2×10⁵ mol/g and a terminal carboxylgroup content of 9.1×10⁵ mol/g. The obtained polyamide blend was fed tothe extruder through the screw type gravimetric feeder (hereinafter,referred to as “feeder 4”) provided at the 1st downstream inlet of theextruder.

The temperature conditions in the extruder were as follows: the 1stcylinder unit was cooled with water, each of the 2nd and 3rd cylinderunits had a temperature of 250° C., each of the 4th to 7th cylinderunits had a temperature of 320° C., each of the 8th to 12th cylinderunits had a temperature of 280° C., and the dye of the extruder had atemperature of 320° C.

The above-mentioned raw materials were melt kneaded together andpelletized using the above-mentioned extruder while adjusting thefeeding rates of the raw materials such that the raw material mixture inthe extruder had a composition as indicated in Table 1 and the dischargerate of the resultant resin composition was 909 kg/h, to thereby obtainpellets of the resin composition.

During the above-mentioned melt-kneading, the screw revolution rate was500 rpm.

(Measurement of the Molecular Weight of Polyphenylene Ether)

About 10 g of the above-obtained pellets were sliced using a microtome,to obtain slices of pellets each having a thickness of about 20 μm. Theobtained slices were extracted with 50 ml of chloroform by using aSoxhlet's extractor, thereby obtaining a solution of sliced pellets inchloroform. The obtained solution of sliced pellets in chloroform (inwhich the main solutes are the polyphenylene ether and the blockcopolymers) was analyzed by GPC (gel permeation chromatography) using anultraviolet spectrometric detector, and the molecular weight ofpolyphenylene ether was determined using a calibration curve obtainedwith respect to the standard polystyrene samples. The ultravioletspectrometric detector was operated at a UV wavelength of 283 nm so asnot to detect the block copolymers which are eluted concomitantly withthe polyphenylene ether during the GPC analysis.

The thus obtained data on the molecular weights were analyzed. As aresult, it was found that the amount of polyphenylene ether moleculeseach independently having a molecular weight of 200,000 or more andpolyphenylene ether molecules each independently having a molecularweight of 5,000 or less were, respectively, 1.45% by weight and 4.78% byweight, each based on the total weight of the polyphenylene ethermolecules. It was also found that the weight ratio of the polyphenyleneether molecules each independently having a molecular weight of 200,000or more to the polyphenylene ether molecules each independently having amolecular weight of 5,000 or less was 0.30.

(Determination of the Area of Polyamide Exposed on the Surface of aPellet (Polyamide Area Ratio))

The ratio of the surface area of polyamide exposed on the surface of theabove-obtained pellet to the overall surface area of the pellet (i.e.,polyamide area ratio) was determined as follows. A pellet was immersedin a 10% by weight aqueous solution of phosphotungstic acid at 40° C.for 8 hours, to thereby dye the pellet selectively at the polyamideportions thereof. Then, the dyed pellet was recovered from the aqueoussolution, followed by washing with water and drying. A photomicrograph(backscattered electron image) (magnification: ×2,500) of the surface ofthe dyed pellet was taken using a field-emission scanning electronmicroscope (FE-SEM) (model “S-4700”; manufactured and sold by Hitachi,Ltd., Japan), wherein the microscope was operated at an accelerationvoltage of 5 kV and the photomicrograph was taken at an angleperpendicular to the surface portion of the pellet, which was observedunder the microscope. With respect to the thus obtained photomicrograph(backscattered electron image), the total area of white portions thereofwas measured using an image analysis device (model name: Image-Pro PLUSver.4.0; Media Cybernetics, Inc., U.S.A.), and the ratio of the totalarea of the white portions to the overall area of the photomicrograph ofthe pellet was obtained as the area of polyamide exposed on the surfaceof the pellet. The result is shown in Table 1. (In the measurement ofthe total area of the white portions in the backscattered electronimage, the threshold for monochromization of the image was determined asfollows. From the histogram of the color tone of the backscatteredelectron image, an intensity of a peak attributed to the color of whiteand an intensity of a peak attributed to the color of black weredetermined, and the mean value of the two intensities was used as thethreshold for monochromization.)

(Matteness of the Surface of a Shaped Resin Article)

Using an injection molding machine “IS80EPN” (cylinder temperature: 280°C.; mold temperature: 80° C.), the above-obtained pellets were moldedinto a shaped resin article in the form of a flat plate having a widthof 50 mm, a length of 90 mm and a thickness of 2.5 mm. The injectionconditions were as follows: the injection velocity (in terms of anaverage velocity of a molten resin passing through the criticalcross-sectional area as prescribed in ISO 294-1) was 200 mm/s, theinjection pressure was a minimum pressure needed to charge a resin intothe molding machine (i.e., minimum pressure needed to prevent a shapedresin article from suffering a sink mark or to prevent the mold frombeing insufficiently filled), the injection time was 20 seconds, and thecooling time was 25 seconds.

The surface of the above-obtained shaped resin article was visuallyobserved. As a result, it was found that almost entire surface of theshaped resin article (except for a portion thereof corresponding to agate of the mold) was matte. In the present invention, the matteness ofthe surface of a shaped resin article is evaluated in accordance withthe following criteria.

I: The entire surface of the shaped resin article has gloss, and thereis almost no matte portion in the surface of the shaped resin article.

II: The shaped resin article has a matte portion only at a surfaceportion thereof corresponding to a point in the mold at which a flow ofa molten resin stops.

III: Almost entire surface of the shaped resin article, except for aportion thereof corresponding to a gate of the mold, is matte.

IV: Almost entire surface of the shaped resin article is matte.

For rendering easy the uniform application of a coating composition onthe surface of a shaped resin article so as to form a coating having auniform thickness, it is preferred that the area of matte portion in thesurface of the shaped resin article is as large as possible.

(Evaluation of the Coating Adhesion Strength)

For evaluation of the strength of adhesion of a coating to a shapedresin article, the above-mentioned flat plate was coated by using anautomated spray coating machine under conditions wherein the resultantcoating had a thickness of 20 μm. As a coating composition, Z-NY (tradename; manufactured and sold by Origin Electric Co., Ltd., Japan) wasused. After completion of the spray coating, the coated flat plate wasbaked at 80° C. for 30 minutes.

Then, the coated flat plate was allowed to stand still at 23° C. and ata humidity of 50% for 24 hours. With respect to a certain area (having asize of 2 cm×2 cm) of the coated surface of the flat plate, the coatedsurface was cut with a cutter to form a checkered cut pattern composedof 100 square coating sections each having a size of 2 mm×2 mm, and apeeling test was performed in which a cellophane adhesive tape wasadhered to the coated surface portion having the checkered cut patternand, then, quickly peeled off. The coating adhesion strength wasevaluated by measuring the number of square coating sections which wereleft on the coated surface after the cellophane adhesive tape had beenpeeled off. As a result, it was found that 95 square coating sections(out of 100 square coating sections) were left on the surface of theflat plate.

The results are shown in Table 1.

(Sharpness of an Image Reflected in the Coated Surface)

The appearance of the above-mentioned coated flat plate was observed asfollows. First, the coated surface of the coated flat plate wascarefully observed to see whether or not there was any unevenness on thesurface. Then, the sharpness of an image reflected in the coated surfacewas evaluated by observing an image of a fluorescent light (locatedabout 1.5 m above the coated flat plate) reflected in the coated surfaceof the flat plate. The criteria for the evaluation are as follows.

Class A: The outline of the image of the fluorescent light reflected inthe coated surface is clearly distinct.

Class B: The outline of the image of the fluorescent light reflected inthe coated surface is indistinct but is recognizable.

Class C: The outline of the image of the fluorescent light reflected inthe coated surface is indistinct and is barely recognizable.

Class D: There are minor unevennesses on the coated surface.

Further, for the purpose of measuring the melt viscosity of a resincomponent forming a dispersed phase of a shaped resin article(hereinafter, referred to as “dispersed phase resin component”), pelletsformed only of the dispersed phase resin component are produced insubstantially the same manner as mentioned above in connection with theproduction of the pellets of the resin composition, except that thefeeding through the 4th feeder was not performed (i.e., only thefeedings through the 1st to 3rd feeders were performed). On the otherhand, for the purpose of measuring the melt viscosity of a resincomponent forming a continuous phase of a shaped resin article(hereinafter, referred to as “continuous phase resin component”),pellets formed only of the continuous phase resin component wereproduced in substantially the same manner as mentioned above inconnection with the production of the pellets of the resin composition,except that the feedings through 1st to 3rd feeders were not performed(i.e., only the feeding through the 4th feeder was performed).

Using the thus obtained pellets, the melt viscosity (ηd) of thedispersed phase resin component and the melt viscosity (ηm) of thecontinuous phase resin component were measured at 290° C. and at a flowrate of 1,000 sec⁻¹ by using a capillary rheometer. As a result, it wasfound that the melt viscosity (ηd) of the dispersed phase resincomponent was about 1,570 Pa·sec, and the melt viscosity (ηm) of thecontinuous phase resin component was about 50 Pa·sec. The ratio((ηd)/(ηm)) between the above-mentioned viscosity values was about 31.

EXAMPLES 2 TO 4 AND COMPARATIVE EXAMPLE 1

The production of pellets of a resin composition was performed insubstantially the same manner as in Example 1, except that the types andamounts of raw materials were changed as shown in Table 1. Table 1 alsoshows the various properties of the obtained pellets, which wereevaluated in substantially the same manner as in Example 1.

Specifically, with respect to the raw materials used in Examples 2 to 4and Comparative Example 1, the raw materials which are different fromthose used in Example 1 are as follows:

Polyphenylene ether powder (hereinafter, referred to as “PPE2”) having areduced viscosity of 0.42 dl/g;

MPPE Produced in Production Example 1;

Polyamide 6,6 (hereinafter, referred to as “PA66-c”) having a viscositynumber of 230 ml/g, a terminal amino group content of 2.4×10⁵ mol/g anda terminal carboxyl group content of 4.8×10⁵ mol/g; and

PA66/6I produced in Production Example 2. TABLE 1 Ex. 1 Ex. 2 Ex. 3 Ex.4 Comp. Ex. 1 Upstream inlet Feeder 1 PPE-1 (parts by weight) *1 38 3830 38 PPE-2 (parts by weight) *2 38 Feeder 2 MPPE (parts by weight) *3 8MAH (parts by weight) *4 0.2 0.3 0.3 0.3 Feeder 3 SEBS1 (parts byweight) *5 4 4 4 4 4 SEBS2 (parts by weight) *6 8 8 8 8 8 1st downstreaminlet Feeder 4 PA66-a (parts by weight) *7 40 40 40 40 PA66-b (parts byweight) *8 10 10 PA66-c (parts by weight) *9 10 50 PA66/6I (parts byweight) *10 10 Polyamide area ratio % 84 94 90 87 67 PPE having amolecular weight of 5,000 % 4.78 — 7.18 3.67 — or less PPE having amolecular weight of 200,000 % 1.45 — 0.82 3.4 — or less PPE having amolecular weight of 200,000 — 0.30 — 0.11 0.93 — or less/PPE having amolecular weight of 50,000 or less Coating adhesion strength (number ofsquare 95 100 60 100 5 coating sections left on the surface of a shapedresin article out of 100 square coating sections) Sharpness of an imagereflected in the coated — A A A A A surface Matteness of the coatedsurface — III II II III I*1 PPE powder having a reduced viscosity of 0.52 dl/g*2 PPE powder having a reduced viscosity of 0.42 dl/g*3 MAH-modified PPE obtained by melt kneading PPE having a reducedviscosity of 0.42 dl/g with MAH*4 Maleic anhydride (in the form of tablets)*5 SEBS block copolymer (styrene content: 33%; Mn: 246,000)*6 SEBS block copolymer (styrene content: 29%; Mn: 98,500)*7 PA6,6 viscosity number: 120 ml/g; [NH₂] = 2.5 × 10⁵ mol/g; [COOH] =11.6 × 10⁵ mol/g*8 PA6,6 viscosity number: 130 ml/g; [NH₂] = 4.2 × 10⁵ mol/g; [COOH] =9.1 × 10⁵ mol/g*9 PA6,6 viscosity number: 230 ml/g; [NH₂] = 2.4 × 10⁵ mol/g; [COOH] =4.8 × 10⁵ mol/g*10 PA6,6/6, I containing 19 mol % of polyamide 6I; [NH₂] = 3.9 × 10⁵mol/g; [COOH] = 10.2 × 10⁵ mol/g

EXAMPLES 5 TO 7 AND COMPARATIVE EXAMPLE 2

The production of pellets of a resin composition was performed insubstantially the same manner as in Example 1, except that thebelow-mentioned raw materials were used. With respect to the obtainedpellets, various properties thereof were measured in substantially thesame manner as in Example 1. The results are shown in Table 2, togetherwith the compositions of the pellets.

Polystyrene/polyethylene butylene/polystyrene block copolymer (styrenecontent: 60%)(hereinafter, referred to as “SEBS3”) having a numberaverage molecular weight (Mn) of 105,000;

ketjen black “EC-600JD” (trade name; manufactured and sold by KetjenBlack International Company Ltd., Japan)(hereinafter, referred to as“KB”); and

polyamide/carbon masterbatch (hereinafter, referred to as “PA-MB”)produced in Production Example 3. TABLE 2 Comp. Ex. 5 Ex. 2 Ex. 6 Ex. 7Upstream inlet Feeder 1 PPE-1 (parts by weight) 38 38 38 22 Feeder 2MPPE (parts by weight) 16 MAH (parts by weight) 0.3 0.3 0.3 Feeder 3SEBS1 (parts by weight) 12 12 3 SEBS2 (parts by weight) 12 5 SEBS3(parts by weight) *11 4 1st downstream inlet Feeder 4 PA66-a (parts byweight) 50 20 PA66-b (parts by weight) 30 30 10 PA66-c (parts by weight)PA-MB (parts by weight) *12 20 20 20 KB (parts by weight) *13 2Polyamide area ratio % 81 75 96 97 PPE having a molecular weight of5,000 % — — — 3.12 or less PPE having a molecular weight of 200,000 % —— — 0.92 or less PPE having a molecular weight of 200,000 — — — — 0.29or less/PPE having a molecular weight of 50,000 or less Coating adhesionstrength (number of square 83 45 70 100 coating sections left on thesurface of a shaped resin article out of 100 square coating sections)Sharpness of an image reflected in the coated — B A B A surfaceMatteness of the coated surface — III II IV IV*11 SEBS block copolymer (styrene content: 60%; Mn: 105,000)*12 Conductive polyamide/carbon masterbatch (carbon content: 10 wt %)*13 Conductive carbon (ketjen black EC600JD)

EXAMPLES 8 TO 10 AND COMPARATIVE EXAMPLE 3

The production of pellets of a resin composition was performed insubstantially the same manner as in Example 1, except that the extruderused in Examples 8 to 10 and Comparative Examples 3 further had anotherscrew type gravimetric feeder (hereinafter, referred to as “feeder 5”)provided at the 2nd downstream inlet through which wollastonite was fedto the extruder, to thereby obtain pellets. With respect to the obtainedpellets, various properties thereof were measured in substantially thesame manner as in Example 1. The results are shown in Table 3, togetherwith the compositions of the pellets. Specifically, with respect to theraw materials used in Examples 8 to 10 and Comparative Example 3, theraw materials which are different from those used in Example 1 or werenot used in Example 1 are as follows:

polyamide 6 “1013B” (trade name; manufactured and sold by UbeIndustries, Ltd., Japan)(hereinafter, referred to as “PA6”); and

the following wollastonites each manufactured and sold by Nyco mineralsInc., U.S.A.:

[wollastonite 1] (average particle diameter: 5 μm, aspect ratio: 13),

[wollastonite 2](average particle diameter: 5 μm, aspect ratio: 3), and

[wollastonite 3] (average particle diameter: 10 μm, aspect ratio: 13)(treated with a 0.5% by weight aminosilane compound). TABLE 3 Comp. Ex.8 Ex. 9 Ex. 3 Ex. 10 Upstream inlet Feeder 1 PPE-1 (parts by weight) 3838 38 38 Feeder 2 MAH (parts by weight) 0.3 0.3 0.3 0.3 Feeder 3 SEBS1(parts by weight) 12 12 12 SEBS2 (parts by weight) 12 1st downstreaminlet Feeder 4 PA66-a (parts by weight) 30 30 30 30 PA6 (parts byweight) 20 PA66/6I (parts by weight) 20 20 20 2nd downstream inletFeeder 5 Wollastonite 1 (parts by weight) *14 20 20 15 Wollastonite 2(parts by weight) *15 5 Wollastonite 3 (parts by weight) *16 20Polyamide area ratio % 87 83 82 88 Coating adhesion strength (number ofsquare coating 100 100 32 100 sections left on the surface of a shapedresin article out of 100 square coating sections) Sharpness of an imagereflected in the coated — A A D A surface Matteness of the coatedsurface — III III I IV*14 Wollastonite (average particle diameter: 5 μm, aspect ratio: 13)*15 Wollastonite (average particle diameter 5 μm, aspect ratio: 3)*16 Wollastonite (average particle diameter: 10 μm, aspect ratio: 13)

EXAMPLE 11

The production of pellets of a resin composition was performed insubstantially the same manner as in Example 1, except that the rawmaterials were used in a proportion as shown in Table 4. With respect tothe obtained pellets, various properties thereof were measured insubstantially the same manner as in Example 1. The results are alsoshown in Table 4, together with the compositions of the pellets. TABLE 4Ex. 11 Upstream inlet Feeder 1 PPE-1 (parts by weight) 38 Feeder 2 MAH(parts by weight) 0.3 Feeder 3 SEBS1 (parts by weight) 3 SEBS2 (parts byweight) 5 SEBS3 (parts by weight) 4 1st downstream inlet PA66-a (partsby weight) 20 PA66-b (parts by weight) 10 PA-MB (parts by weight) 20 2nddownstream inlet Wollastonite 1 (parts by 15 weight) Wollastonite 2(parts by 5 weight) Wollastonite 3 (parts by weight) Polyamide arearatio % 92 Coating adhesion strength (number of square 100 coatingsections left on the surface of a shaped resin article out of 100 squarecoating sections) Sharpness of an image reflected in — A the coatedsurface Matteness of the coated surface — IV

INDUSTRIAL APPLICABILITY

The shaped resin article of the present invention is advantageous notonly in that the shaped resin article has excellent matte surface, butalso in that the shaped resin article has excellent strength of adhesionto a coating formed on the shaped resin article (i.e., “coating adhesionstrength”), and such a coating formed on the shaped resin article hasexcellent sharpness of an image reflected therein (i.e., the coating hasexcellent luster). Further, by the use of the conductive resincomposition of the present invention, it becomes possible to produce ashaped article which is advantageous not only in that the shaped articlehas excellent matte surface, but also in that the shaped article hasexcellent coating adhesion strength, and a coating formed on the shapedarticle has excellent sharpness of an image reflected therein. Inaddition, the produced shaped article has a satisfactorily lowcoefficient of linear expansion, which is especially advantageous in thefield of large shaped articles, such as an automobile fender and anautomobile back door. The shaped resin article of the present inventionand the shaped article produced from the conductive resin composition ofthe present invention can be advantageously used in a wide variety offields, e.g., not only in a field of exterior parts for automobiles, butalso in the fields of electric and electronic parts, parts of officeautomation machines, mechanical parts, and electric and interior partsof motorcycles and automobiles.

1. A shaped resin article comprising: a polyamide (A) comprising atleast two different polyamide components, a polyphenylene ether (B), andone or more partially hydrogenated block copolymers (C), eachindependently obtained by partially hydrogenating an unhydrogenatedblock copolymer comprising at least one aromatic vinyl polymer blockcomprised mainly of aromatic vinyl monomer units, and at least oneconjugated diene polymer block comprised mainly of conjugated dienemonomer units, said partially hydrogenated block copolymers (C)including at least one partially hydrogenated block copolymer (C-1)having a number average molecular weight of from 200,000 to 300,000,wherein said polyamide (A) is present as a continuous phase in whichsaid polyphenylene ether (B) is dispersed to form a dispersed phase, andsaid partially hydrogenated block copolymer (C) is present in at leastone phase selected from the group consisting of said continuous phase ofthe polyamide (A) and said dispersed phase of the polyphenylene ether(B), wherein said polyamide (A) is exposed on a surface of said shapedresin article so that the surface area of the polyamide (A) exposed onthe overall surface of said shaped resin article is at least 80%, basedon the surface area of the shaped resin article.
 2. The shaped resinarticle according to claim 1, wherein said polyamide (A) comprises atleast two different polyamide components having their respectivedifferent viscosities.
 3. The shaped resin article according to claim 1,wherein said component (A) comprises polyamide 6,6 and a polyamide otherthan polyamide 6,6.
 4. The shaped resin article according to claim 3,wherein said polyamide other than polyamide 6,6 is polyamide
 6. 5. Theshaped resin article according to claim 3, wherein said polyamide otherthan polyamide 6,6 is a polyamide comprising recurring units, eachindependently represented by the following formula (1):

wherein each of R¹ and R² independently represents a C₃-C₁₄ alkylenegroup or a C₆-C₉ arylene group, with the proviso that R¹ and R² are notsimultaneously a C₆ alkylene group or a C₆ arylene group.
 6. The shapedresin article according to claim 1, wherein said polyamide (A) comprisesat least one polyamide component having a terminal amino group contentof from 1×10⁻⁵ mol/g to 4×10⁻⁵ mol/g.
 7. The shaped resin articleaccording to claim 1, wherein said polyphenylene ether (B) containsrelatively high molecular weight polyphenylene ether molecules, eachindependently having a molecular weight of 200,000 or more, andrelatively low molecular weight polyphenylene ether molecules, eachindependently having a molecular weight of 5,000 or less, wherein theweight ratio of said relatively high molecular weight polyphenyleneether molecules to said relatively low molecular weight polyphenyleneether molecules is 0.35 or less.
 8. The shaped resin article accordingto claim 1, wherein said polyphenylene ether (B) contains relativelyhigh molecular weight polyphenylene ether molecules, each independentlyhaving a molecular weight of 200,000 or more, and relatively lowmolecular weight polyphenylene ether molecules, each independentlyhaving a molecular weight of 5,000 or less, wherein the amount of saidrelatively low molecular weight polyphenylene ether molecules and theamount of said relatively high polyphenylene ether molecules are,respectively, 5% by weight or less and 2% by weight or less, based onthe weight of said polyphenylene ether resin (B).
 9. The shaped resinarticle according to claim 1, wherein said one or more partiallyhydrogenated block copolymers (C) further include at least one partiallyhydrogenated block copolymer (C-2) having a number average molecularweight of from 50,000 to 150,000.
 10. The shaped resin article accordingto claim 9, wherein said at least one partially hydrogenated blockcopolymer (C-1) and said at least one partially hydrogenated blockcopolymer (C-2) collectively include: at least one partiallyhydrogenated block copolymer having a high aromatic vinyl monomer unitcontent, which is obtained by partially hydrogenating an unhydrogenatedblock copolymer in which said at least one aromatic vinyl polymer blockis present in an amount of from 60 to 90% by weight, based on the weightof said unhydrogenated block copolymer, and at least one partiallyhydrogenated block copolymer having a low aromatic vinyl monomer unitcontent, which is obtained by partially hydrogenating an unhydrogenatedblock copolymer in which said at least one aromatic vinyl polymer blockis present in an amount of from 20 to less than 60% by weight, based onthe weight of said unhydrogenated block copolymer, and wherein the totalamount of the aromatic vinyl polymer blocks present in said hydrogenatedblock copolymers (C-1) and (C-2) is 30 to 40% by weight, based on thetotal weight of said hydrogenated block copolymers (C-1) and (C-2). 11.The shaped resin article according to claim 1, which further comprisesat least one carbonaceous material (D) selected from the groupconsisting of a conductive carbon black, carbon fibers and carbonnanotubes, and which is produced by melt-kneading a masterbatchcomprising said polyamide (A) having dispersed therein said carbonaceousmaterial (D) with said polyphenylene ether (B), said one or morepartially hydrogenated block copolymers (C), and optionally at least onemember selected from the group consisting of an additional amount ofsaid polyamide (A) and an additional amount of said carbonaceousmaterial (D).
 12. The shaped resin article according to claim 1, whichfurther comprises (E) wollastonite particles having an average particlediameter of from 2 to 9 μm.
 13. The shaped resin article according toclaim 12, wherein said wollastonite particles (E) have at least twodifferent aspect ratios.
 14. The shaped resin article according to claim1, which is a pellet.
 15. The shaped resin article according to claim 1,which is an automobile exterior part.
 16. A conductive resin compositioncomprising: a polyamide (A), a polyphenylene ether (B), a blockcopolymer (C) comprising at least one aromatic vinyl polymer blockcomprised mainly of aromatic vinyl monomer units, and at least oneconjugated diene polymer block comprised mainly of conjugated dienemonomer units, a conductive carbonaceous material (D), and wollastoniteparticles (E).
 17. The conductive resin composition according to claim16, which is produced by melt-kneading a masterbatch comprising saidpolyamide (A) having dispersed therein said carbonaceous material (D)with said polyphenylene ether (B), said one or more partiallyhydrogenated block copolymers (C), said wollastonite particles (E), andoptionally at least one member selected from the group consisting of anadditional amount of said polyamide (A) and an additional amount of saidcarbonaceous material (D), and wherein said carbonaceous material (D) isat least one member selected from the group consisting of a conductivecarbon black, carbon fibers and carbon nanotubes.
 18. The conductiveresin composition according to claim 16, wherein said wollastoniteparticles (E) have an average diameter of from 2 to 9 μm.
 19. Theconductive resin composition according to claim 16, wherein saidwollastonite particles (E) include particles having an aspect ratio of 5or more and particles having an aspect ratio of less than 5, wherein theamount of said wollastonite particles (E) having an aspect ratio of 5 ormore is 50% by weight or more, based on the total weight of thewollastonite particles (E).